Shuqiang Jiao

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Organization: University of Science and Technology Beijing
Department: State Key Laboratory of Advanced Metallurgy
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Co-reporter:Shuqiang Jiao, Jingjing Tuo, Hongliang Xie, Zihang Cai, Shuai Wang, Jun Zhu
Materials Research Bulletin 2017 Volume 86() pp:194-200
Publication Date(Web):February 2017
DOI:10.1016/j.materresbull.2016.10.019
•Cu3[Fe(CN)6]2 powders were synthesized simply by solution precipitation method.•The material can intercalate Na+ reversibly at high potential plateaus around 3.32 V.•The material can realize the single electron redox capacity due to the reduction of ferric-ion.Prussian blue analogues (PBAs) have recently attracted extensive interests as a new class of cathode materials for rechargeable batteries. Copper hexacyanoferrate, a typical Prussian blue analogue with the chemical formula Cu3[Fe(CN)6]2, has been synthesized by solution precipitation method and investigated as a cathode material for sodium-ion batteries. The galvanostatic cycling tests show a specific capacity of 44 mA h g−1 at a current density of 20 mA g−1, and the capacity retention can be 57.1% after 50 cycles. The material can also deliver a specific capacity of 37 mA h g−1 and 25 mA h g−1 at a rate of 50 mA g−1 and 100 mA g−1, respectively. Furthermore, the material exhibits a high reduction peak at 3.32 V vs. Na+/Na, which brings more power to sodium-ion batteries. The data indicate the as-prepared material is capable of realizing the single electron redox capacity due to the reduction of Fe3+/Fe2+. All of the findings suggest a possible use of Cu3[Fe(CN)6]2 nanoparticles as environmental friendly and cost-effective cathode material, which also open new perspectives to develop cathode materials for sodium-ion batteries.
Co-reporter:Jiguo Tu;Kai Wu;Hui Tang;Henghui Zhou
Journal of Materials Chemistry A 2017 vol. 5(Issue 32) pp:17021-17028
Publication Date(Web):2017/08/15
DOI:10.1039/C7TA04426G
The development of fast-charging lithium-ion batteries (LIBs) is an urgent necessity. Nevertheless, it is still a huge challenge to prepare superior high-rate cathode materials for LIBs. In this work, porous Mg–Ti co-doped LiFe0.985Mg0.005Ti0.01PO4 microspheres are successfully synthesized via a carbothermic reduction reaction in combination with a spray drying process, with FePO4 as the Fe and P source. Through X-ray diffraction (XRD) combined with X-ray photoelectron spectroscopy (XPS) Ar+-sputtering technology, it confirms that Mg and Ti are in the form of doping rather than surface recombination inside LiFePO4 microspheres, and the existence of Fe3+ inside the samples is confirmed as residual FePO4. Compared to the undoped sample, the porous Mg–Ti co-doped LiFePO4 microspheres show great improvement in electronic conductivity (1.58 × 10−3 S cm−1) and diffusion coefficient (5.97 × 10−9 cm s−1 for charging and 4.30 × 10−9 cm s−1 for discharging). More importantly, the porous Mg–Ti co-doped LiFe0.985Mg0.005Ti0.01PO4 microspheres show excellent high-rate capabilities, delivering a discharge capacity of 161.5, 160.3, 156.7, 147.5, 139.8 and 131.5 mA h g−1 at 0.2C, 0.5C, 1C, 3C, 5C and 8C, respectively.
Co-reporter:Zepeng Kang;Kailong Jiao;Ruiyun Peng;Zongqian Hu
RSC Advances (2011-Present) 2017 vol. 7(Issue 20) pp:11872-11879
Publication Date(Web):2017/02/16
DOI:10.1039/C7RA00852J
Herein, we report the first example of using the Al-based porous coordination polymers (Al-PCP) as a template for preparation of nanoporous carbon through a two-step carbonized method. By applying the appropriate carbonized temperature in the first-step carbonization process, both high surface area and large pore volume are realized in the second-step carbonization process even at a high-temperature. The SEM images show that the carbonized Al-PCP before and after HF treatment (PCP) retained mostly crystallite shapes and sponge-like surface morphology. The TEM images of carbonized Al-PCP and PCP clearly exhibited high porosity with a wide range of pore sizes spanning from micro- to macropores. The maximum BET surface area and pore volume were 2773.5 m2 g−1 and 1.885 cm3 g−1, respectively. The obtained highly nanoporous carbon PCPs were used to modify a glassy carbon electrode (GCE) based on glucose oxidase (GOx), resulting in efficient direct electron transfer and excellent bio-catalytic performance. In addition, a glucose/O2 fuel cell constructed using Nafion/GOx/PCP/GCE as the anode and an E-TEK Pt/C modified GCE as the cathode generated a maximum power density of 0.548 mW cm−2 at 0.41 V. The findings in this work may be helpful for exploiting novel nanoporous carbons derived from metal–organic framework (MOF) by using a two-step carbonization method for the immobilization of enzymes in enzymatic biofuel cells or biosensors.
Co-reporter:Shuai Wang;Donghua Tian;Hao-Sen Chen;Hong Jiao;Jiguo Tu;Yingjun Liu;Dai-Ning Fang
Advanced Materials 2017 Volume 29(Issue 16) pp:
Publication Date(Web):2017/04/01
DOI:10.1002/adma.201606349
An ultrafast rechargeable multi-ions battery is presented, in which multi-ions can electrochemically intercalate into graphite layers, exhibiting a high reversible discharge capacity of ≈100 mAh g−1 and a Coulombic efficiency of ≈99% over hundreds of cycles at a high current density. The results may open up a new paradigm for multi-ions-based electrochemical battery technologies and applications.
Co-reporter:Zepeng Kang, Kailong Jiao, Xinping Xu, Ruiyun Peng, Shuqiang Jiao, Zongqian Hu
Biosensors and Bioelectronics 2017 Volume 96(Volume 96) pp:
Publication Date(Web):15 October 2017
DOI:10.1016/j.bios.2017.05.025
•A 3D architecture of PANI@GO composite was synthesized via in-situ polymerization and then carbonized at 1600 °C.•Nanofiber-like PANI on the GO surface was mostly preserved after carbonization.•Carbonized PANI grew seamlessly on the GO surface and served as a conductive “network”.•The Ks of fabricated electrode based on PANI1600@GO and GOx was 13.03 s-1.A three-dimensional architecture of PANI@GO hybrid was synthesized via in-situ polymerization of aniline monomers on the surface of graphene oxide (GO) and carbonized at 1600 °C. The SEM images showed that surfaces of planar GO were covered by a compact nanofiber-like polyaniline (PANI) layer which presented an interconnected network. Nanofiber-like PANI on the GO surface was mostly preserved and became the carbon nanofibers (CNFs) after carbonization. The TEM images showed that the carbonized PANI grew seamlessly on the GO surface and served as conductive “network” between interlayers of GO. The carbonized PANI@GO hybrid was used to modify a glassy carbon electrode (GCE) based on GOx, resulting in efficient direct electron transfer (DET) and excellent bio-catalytic performance. In addition, a glucose/O2 fuel cell constructed using Nafion/GOx/PANI1600@GO/GCE as the anode and an E-TEK Pt/C modified GCE as the cathode generated a maximum power density of 0.756 mW cm−2 at 0.42 V. Findings in this study may be helpful for exploiting novel materials for immobilization of enzymes through carbonizing conducting polymers or their composites with inorganic materials at high temperature for applications in enzymatic biofuel cells or biosensors.
Co-reporter:Chen Wang;Junfeng Li;Handong Jiao;Jiguo Tu
RSC Advances (2011-Present) 2017 vol. 7(Issue 51) pp:32288-32293
Publication Date(Web):2017/06/21
DOI:10.1039/C7RA05860H
Due to its characteristics of high capacity, low cost, being non-flammable, and involving a three-electron-redox reaction, the aluminum rechargeable battery has received wide attention. Because of these advantages, we focus on a low-cost aluminum alloy anode and detect the discharge/charge reaction mechanism in the aluminum chloride-urea liquid electrolyte at 110–130 °C. The discharge voltage of the battery is about 1.9 V and 1.6 V, and at the current density of 100 mA g−1 the cell can produce a specific capacity of ∼94 mA h g−1. Compared to the pure aluminum anode, the system has a promising future for high efficiency, low-cost energy storage devices.
Co-reporter:Zepeng Kang;Kailong Jiao;Chao Yu;Ji Dong;Ruiyun Peng;Zongqian Hu
RSC Advances (2011-Present) 2017 vol. 7(Issue 8) pp:4572-4579
Publication Date(Web):2017/01/10
DOI:10.1039/C6RA26636C
Due to their unique physicochemical properties, carbon nanochips (CNCs) have been used for studies of the direct electrochemical and electrocatalytic properties of oxidoreductase. In this report, a glassy carbon electrode (GCE) was modified with CNCs, and glucose oxidase (GOx) was immobilized on the modified electrode surface. Chitosan (CS) was employed to fix the GOx/CNCs tightly to the surface of the GCE. Characterization of the modified electrode by SEM, TEM, and FT-IR showed that GOx remained in its native structure when immobilized in CNC film. The results of electrochemical impedance spectroscopy, cyclic voltammetry, and linear sweep voltammetry studies showed that direct electrochemical and bioelectrocatalytic activities of GOx were achieved and that the presence of CNCs enhanced the electrochemical response of GOx. Glucose had a linear current response from 0 to 1.9 mM, with a detection limit of 0.16 mM and an apparent Michaelis–Menten constant of 0.15 mM. The polarization curve of the biofuel cell revealed that the bioanode afforded an open circuit voltage of 0.59 V, maximum power density of 55 μW cm−2, and maximum current density of 434 μA cm−2. These results establish that the direct immobilization of protein onto the CNC surface can be used to achieve direct electron transfer of other redox enzymes. Furthermore, the findings provide a new perspective toward understanding the kinetics and thermodynamics of biological redox processes.
Co-reporter:Yang Song;Jiguo Tu;Junxiang Wang;Yingjun Liu;Handong Jiao;Xuhui Mao;Zhancheng Guo;Derek J. Fray
Journal of Materials Chemistry A 2017 vol. 5(Issue 3) pp:1282-1291
Publication Date(Web):2017/01/17
DOI:10.1039/C6TA09829K
Affordable and scalable energy storage systems are necessary to mitigate the output fluctuation of an electrical power grid integrating intermittent renewable energy sources. Conventional battery technologies are unable to meet the demanding low-cost and long-life span requirements of a grid-scale application, although some of them demonstrated impressive high energy density and capacity. More recently, the prototype of an Al-ion battery has been developed using cheap electrode materials (Al and graphite) in an organic room-temperature ionic liquid electrolyte. Here we implement a different Al-ion battery in an inorganic molten salt electrolyte, which contains only an extremely low-cost and nonflammable sodium chloroaluminate melt working at 120 °C. Due to the superior ionic conductivity of the melt electrolyte and the enhanced Al-ion interaction/deintercalation dynamics at an elevated temperature of 120 °C, the battery delivered a discharge capacity of 190 mA h g−1 at a current density of 100 mA g−1 and showed an excellent cyclic performance even at an extremely high current density of 4000 mA g−1: 60 mA h g−1 capacity after 5000 cycles and 43 mA h g−1 capacity after 9000 cycles, with a coulombic efficiency constantly higher than 99%. The low-cost and safe characteristics, as well as the outstanding long-term cycling capability at high current densities allow the scale-up of this brand-new battery for large-scale energy storage applications.
Co-reporter:Liwen Hu;Yang Song;Jianbang Ge;Jun Zhu;Zhenchao Han
Journal of Materials Chemistry A 2017 vol. 5(Issue 13) pp:6219-6225
Publication Date(Web):2017/03/28
DOI:10.1039/C7TA00258K
As part of the efforts to address global climate change, the identification of methods for the capture of carbon dioxide and its selective electrochemical conversion into value-added carbonaceous materials in molten salt electrolytes is a research topic of scientific and technological significance. In most cases, metal electrodes such as nickel and stainless steel are used as the cathode to investigate the nucleation and growth of a variety of carbon nanostructures. In this study, the electrochemical deposition of carbon nanotubes (CNTs) and carbon microstructures was performed in molten CaCl2–NaCl–CaO using glassy carbon and graphite rod as the cathode and RuO2–TiO2 as the anode. The capture formula was established and the capture coefficient was defined and calculated to be 1.8 s−1. Cyclic voltammetry, constant voltage electrolysis, as well as on-line outlet gas analysis were conducted to investigate the electrode reactions, and the results indicated that the captured CO2 can be electrochemically converted to carbon and environmentally-friendly oxygen as the only by-product. SEM and TEM images showed that quasi-spherical and nanotubular carbon were deposited on the graphite and glassy carbon cathodes at 750 °C. However, by regulating the temperature, quasi-spheres and nanosheets were observed at the glassy carbon cathode.
Co-reporter:Handong Jiao;Chen Wang;Jiguo Tu;Donghua Tian
Chemical Communications 2017 vol. 53(Issue 15) pp:2331-2334
Publication Date(Web):2017/02/16
DOI:10.1039/C6CC09825H
A new Al-ion battery based on an affordable and nontoxic liquid electrolyte made from molten AlCl3/urea was assembled. As the cathode material, natural graphite shows two well-defined discharge voltage plateaus at about 1.9 and 1.5 V with a high specific capacity of 93 mA h g−1 and excellent coulombic efficiency (>99%). The attractive capacity (about 78 mA h g−1) is retained even at a high current density of 1000 mA g−1. Moreover, no faster fading in capacity is observed after 500 cycles. This electrolyte could provide a new system for Al ion batteries, which can be used for large scale energy storage, owing to its cost advantages, high-rate capability and durability.
Co-reporter:Shuai Wang, Shuqiang JiaoJunxiang Wang, Hao-Sen Chen, Donghua Tian, Haiping Lei, Dai-Ning Fang
ACS Nano 2017 Volume 11(Issue 1) pp:
Publication Date(Web):December 15, 2016
DOI:10.1021/acsnano.6b06446
On the basis of low-cost, rich resources, and safety performance, aluminum-ion batteries have been regarded as a promising candidate for next-generation energy storage batteries in large-scale energy applications. A rechargeable aluminum-ion battery has been fabricated based on a 3D hierarchical copper sulfide (CuS) microsphere composed of nanoflakes as cathode material and room-temperature ionic liquid containing AlCl3 and 1-ethyl-3-methylimidazolium chloride ([EMIm]Cl) as electrolyte. The aluminum-ion battery with a microsphere electrode exhibits a high average discharge voltage of ∼1.0 V vs Al/AlCl4–, reversible specific capacity of about 90 mA h g–1 at 20 mA g–1, and good cyclability of nearly 100% Coulombic efficiency after 100 cycles. Such remarkable electrochemical performance is attributed to the well-defined nanostructure of the cathode material facilitating the electron and ion transfer, especially for chloroaluminate ions with large size, which is desirable for aluminum-ion battery applications.Keywords: aluminum-ion battery; cathode material; copper sulfide; microsphere;
Co-reporter:Jun Zhu;Long Zhang
Metallurgical and Materials Transactions B 2017 Volume 48( Issue 1) pp:286-293
Publication Date(Web):09 September 2016
DOI:10.1007/s11663-016-0812-9
A controllable and facile process for the preparation of Nb3Sn intermetallic compound nanopowders using NbCl5 and SnCl2 vapors reduced by hydrogen has been developed. The vaporizing rates of the two chlorides are controlled by measuring their mass loss as a function of carrier gas (argon) flow rate at certain vaporization temperatures, respectively. X-ray diffraction (XRD) patterns indicate that hydrogenous Nb3Sn products are obtained under the vaporizing rate of 0.155 g min−1 for NbCl5 and 0.036 g min−1 for SnCl2 with the hydrogen flow rate of 2100 ml min−1 at 1273 K (1000 °C). Results of semi-quantitative analysis by X-ray fluorescence (XRF) demonstrate that the atomic ratio of Nb to Sn in the as-synthesized products is 3.48:1, and the content of (Nb + Sn) is taken up to 89.61 wt pct from the total weight of the products. The products can be purified by vacuum heat treatment. Images of transmission electron microscopy (TEM) show that the products are homogenous particles with a mean diameter of 31 nm. In addition, the reaction ratio of the chlorides and the powder yield are controllable by hydrogen flow rate.
Co-reporter:Yang Song;Zhancheng Guo;Zongqian Hu;Junxiang Wang
RSC Advances (2011-Present) 2017 vol. 7(Issue 7) pp:3879-3887
Publication Date(Web):2017/01/09
DOI:10.1039/C6RA24707E
At present, an in situ synthesis of a conductive polyaniline (PANI) film via self-assembly is particularly of great interest in the supercapacitor field. Herein, we report the discovery a nanostructuring process for PANI electrochemical self-assembly through a forced convection method. It was observed that the morphology and structure of PANI films at the nanometer scale could be controlled by varying the rotation speed of the disk electrode during the electropolymerization process. On increasing the rotation speed from 0 rpm to 1000 rpm, the growth of PANI films successively changes from the nanorods composed porous films to the nanoparticles (diameter of 50 nm) composed dense films. We have also demonstrated the efficient electrochemical properties of the electrochemically assembled nano-PANI film-based electrodes at a rotation speed of 100 rpm, which showed the highest capacitance of 700.50 F g−1 at a current density of 1 A g−1 and good cycle stability after 1000 cycles.
Co-reporter:Shuai Wang;Zhijing Yu;Jiguo Tu;Junxiang Wang;Donghua Tian;Yingjun Liu
Advanced Energy Materials 2016 Volume 6( Issue 13) pp:
Publication Date(Web):
DOI:10.1002/aenm.201600137

Due to an ever-increasing demand for electronic devices, rechargeable batteries are attractive for energy storage systems. A novel rechargeable aluminum-ion battery based on Al3+ intercalation and deintercalation is fabricated with Ni3S2/graphene microflakes composite as cathode material and high-purity Al foil as anode. This kind of aluminum-ion battery comprises of an electrolyte containing AlCl3 in an ionic liquid of 1-ethyl-3-methylimidazolium chloride ([EMIm]Cl). Galvanostatic charge/discharge measurements have been performed in a voltage range of 0.1–2.0 V versus Al/AlCl4 . An initial discharge specific capacity of 350 mA h g−1 at a current density of 100 mA g−1 is achieved, and the discharge capacity remains over 60 mA h g−1 and coulombic efficiency of 99% after 100 cycles. Typically, for the current density at 200 mA g−1, the initial charge and discharge capacities are 300 and 235 mA h g−1, respectively. More importantly, it should be emphasized that the battery has a high discharge voltage plateau (≈1.0 V vs Al/AlCl4 ). These meaningful results represent a significant step forward in the development of aluminum-ion batteries.

Co-reporter:Zhijing Yu, Zepeng Kang, Zongqian Hu, Jianhong Lu, Zhigang Zhou and Shuqiang Jiao  
Chemical Communications 2016 vol. 52(Issue 68) pp:10427-10430
Publication Date(Web):26 Jul 2016
DOI:10.1039/C6CC05974K
Hexagonal NiS nanobelts served as novel cathode materials for rechargeable Al-ion batteries based on an AlCl3/[EMIm]Cl ionic liquid electrolyte system. The nano-banded structure of the materials can facilitate the electrolyte immersion and enhance Al3+ diffusion. The hexagonal NiS nanobelt based cathodes exhibit high storage capacity, good cyclability and low overpotential.
Co-reporter:Jianbang Ge, Shuai Wang, Liwen Hu, Jun Zhu, Shuqiang Jiao
Carbon 2016 Volume 98() pp:649-657
Publication Date(Web):March 2016
DOI:10.1016/j.carbon.2015.11.065
Carbon deposition on a W cathode during the electrolysis was performed in molten LiCl–NaCl–Na2CO3 under CO2 atmosphere. The electrochemical process was investigated by cyclic voltammetry on the glass carbon electrode. The minimum energy consumption is 20.1 kWh for 1 kg of carbon. Constant voltage electrolysis combined with a real-time resolution mass spectrum demonstrated the absence of the formation of carbon monoxide even at 800 °C. The carbon products deposited at different electrolysis conditions were composed of amorphous carbon and mainly comprised of quasi-spherical carbon particles accompanied by small amounts of wire-like carbon.
Co-reporter:Shuqiang Jiao, Haiping Lei, Jiguo Tu, Jun Zhu, Junxiang Wang, Xuhui Mao
Carbon 2016 Volume 109() pp:276-281
Publication Date(Web):November 2016
DOI:10.1016/j.carbon.2016.08.027
In this work, a rechargeable Ah-level soft-package aluminum-ion (AIBs) battery is fabricated using carbon paper cathode, high-purity aluminum foil anode and ionic liquid electrolyte consisting of AlCl3 and 1-ethyl-3-methylimidazalium chloride ([EMIm]Cl). It is amazing that the prototype battery, providing a maximal charge of 1.3 Ah at 10 mA g−1 current density, can light LED lamp for 14 h, and prototype battery series can drive a super mini kart steadily. The stable performances of rechargeable Ah-level aluminum-ion battery demonstrate their wide prospects in industrial application. Moreover, we found that the graphitic cathode materials from the used rechargeable AIBs can be completely recycled as graphene products through a facile treatment of electrolysis. The results are significantly meaningful for promoting the industrialized application and the sustainable development of AIBs.
Co-reporter:Yan Yuan, Junxiang Wang, Zongqian Hu, Haiping Lei, Donghua Tian, Shuqiang Jiao
Journal of Alloys and Compounds 2016 Volume 685() pp:344-349
Publication Date(Web):15 November 2016
DOI:10.1016/j.jallcom.2016.05.335
•A Prussian blue analogue has been fabricated by a facile co-precipitation method.•Na2Co3[Fe(CN)6]2 has been studied as an cathode material for lithium-ion and sodium-ion batteries.•The synthesized material has steady cycling performance.A Prussian blue analogue, Na2Co3[Fe(CN)6]2, has been fabricated by a facile co-precipitation method at room temperature as a potential cathode material for both lithium-ion and sodium-ion batteries. It found that the Na2Co3[Fe(CN)6]2 nanoparticles with a primary particle size of 30–40 nm have been synthesized, and exhibited an excellent electrochemical performance, including a long cycling behavior in lithium-ion batteries and a good rate performance in sodium-ion batteries. In lithium-ion batteries, the Na2Co3[Fe(CN)6]2 nanoparticles cathode can deliver an excellent cyclic performance with 73.0% retention of initial capacity after 50 cycles at 50 mA g−1. Moreover, when Na2Co3[Fe(CN)6]2 is used as cathode material of sodium-ion batteries, it exhibits an outstanding rate performance exceeding 75.2% retention of initial capacity after 50 cycles at 200 mA g−1. Therefore, the Na2Co3[Fe(CN)6]2 nanoparticles can be a potential cathode candidate for the application of lithium-ion and sodium-ion batteries due to its excellent electrochemical performance, easy preparation, low cost and environment benefits.
Co-reporter:Handong Jiao, Junxiang Wang, Jianbang Ge, Long Zhang, Hongmin Zhu, Shuqiang Jiao
Solid State Communications 2016 Volumes 231–232() pp:53-56
Publication Date(Web):April 2016
DOI:10.1016/j.ssc.2016.02.003
•Ru-doped LaCrO3 is synthesized by solid-state reaction method.•The dense pellets are obtained by spark plasma sintering.•The synthesized pellet has good conductivity.Ru-doped lanthanum chromates (LaRuxCr1−xO3) were prepared through a solid-state reaction method. The perovskite pellets with high bulk density over 98% were obtained using the as-prepared LaRuxCr1−xO3 powders as starting materials by spark plasma sintering (SPS) process. The pellets performed high electrical conductivity, which increased with increasing of temperature and ruthenium content (0≤x≤0.10). The activation energy of lanthanum chromate was found to be decreased due to the ruthenium doping.
Co-reporter:Liwen Hu;Yang Song;Dr. Shuqiang Jiao;Yingjun Liu;Jianbang Ge;Hong Jiao;Jun Zhu;Junxiang Wang;Dr. Hongmin Zhu;Dr. Derek J. Fray
ChemSusChem 2016 Volume 9( Issue 6) pp:588-594
Publication Date(Web):
DOI:10.1002/cssc.201501591

Abstract

Producing graphene through the electrochemical reduction of CO2 remains a great challenge, which requires precise control of the reaction kinetics, such as diffusivities of multiple ions, solubility of various gases, and the nucleation/growth of carbon on a surface. Here, graphene was successfully created from the greenhouse gas CO2 using molten salts. The results showed that CO2 could be effectively fixed by oxygen ions in CaCl2–NaCl–CaO melts to form carbonate ions, and subsequently electrochemically split into graphene on a stainless steel cathode; O2 gas was produced at the RuO2–TiO2 inert anode. The formation of graphene in this manner can be ascribed to the catalysis of active Fe, Ni, and Cu atoms at the surface of the cathode and the microexplosion effect through evolution of CO in between graphite layers. This finding may lead to a new generation of proceedures for the synthesis of high value-added products from CO2, which may also contribute to the establishment of a low-carbon and sustainable world.

Co-reporter:Shuai Wang, Wei Wang, Pan Zhan, Yan Yuan, Kailong Jiao, Handong Jiao and Shuqiang Jiao  
Journal of Materials Chemistry A 2015 vol. 3(Issue 32) pp:16528-16534
Publication Date(Web):07 Jul 2015
DOI:10.1039/C5TA03160E
The synthesis and electrochemical performance derived from NaHTi3O7 have been investigated for use as an anode material for sodium-ion batteries. NaHTi3O7 nanotubes were fabricated by a hydrothermal method. Galvanostatic charge/discharge measurements were performed in a voltage range of 0.01–2.5 V vs. Na+/Na at different current densities, using the as-prepared NaHTi3O7 nanotubes as the working electrode. Typically, the initial discharge and charge capacities of NaHTi3O7 nanotubes were 381.80 mA h g−1 and 242.82 mA h g−1, respectively, at a current density of 20 mA g−1, and still retained a high specific capacity of 105.32 mA h g−1 and 100.65 mA h g−1 after 100 cycles. The electrode also exhibits outstanding rate capability with a reversible capacity as high as 300.95 mA h g−1 and 209.10 mA h g−1 at current densities of 50 mA g−1 and 100 mA g−1, respectively. The excellent electrochemical stability and high specific capacity of these nanostructured materials have been attributed to the three-dimensional flower-like morphology of NaHTi3O7 nanotubes. All of the findings demonstrate that NaHTi3O7 nanotubes have steady cycling performance and environmental and cost friendliness for use in next generation secondary batteries of sodium-ion batteries.
Co-reporter:Liwen Hu, Yang Song, Jianbang Ge, Jun Zhu and Shuqiang Jiao  
Journal of Materials Chemistry A 2015 vol. 3(Issue 42) pp:21211-21218
Publication Date(Web):09 Sep 2015
DOI:10.1039/C5TA05127D
Molten CaCl2 is reported to be a potential dopant for reactivation of CaO and enhancement of the cyclic capture ability of CaO. The present work showed that O2− in molten CaCl2–CaO has a strong affinity for CO2 at 850 °C, with resulting formation of carbonates. Using a RuO2·TiO2 inert anode, the formed carbonates were successfully electrochemically split into value-added ultrathin graphite sheets, which look like a kind of graphene, accompanied by evolution of carbon monoxide at the cathode and environmentally friendly by-product oxygen at the anode. The reduction mechanism of CO32− was investigated by cyclic voltammetry and square wave voltammetry. Results demonstrated that there are two steps in electrochemical reduction of CO32−, and the transferred electron numbers calculated for each step are 1.76 and 1.99, respectively. The kind of graphene generated at the cathode may have applications in fields such as energy storage and electronic devices. The molten CaCl2–CaO has potential applications and prospects in large-scale capture of CO2, and electrochemical conversion of CO2 into high value added carbon material such as ultrathin graphite sheets with renewable energy sources.
Co-reporter:Haobo Sun, Wei Wang, Zhijing Yu, Yan Yuan, Shuai Wang and Shuqiang Jiao  
Chemical Communications 2015 vol. 51(Issue 59) pp:11892-11895
Publication Date(Web):16 Jun 2015
DOI:10.1039/C5CC00542F
A new kind of Al-ion battery with carbon paper as the cathode, high-purity Al foil as the anode and ionic liquid as the electrolyte is proposed in this work. The significance of the presented battery is going to be an extremely high average voltage plateau of ca. 1.8 V vs. Al3+/Al.
Co-reporter:Liwen Hu, Zhijing Yu, Zongqian Hu, Yang Song, Feng Zhang, Hongmin Zhu, Shuqiang Jiao
Electrochimica Acta 2015 Volume 174() pp:273-281
Publication Date(Web):20 August 2015
DOI:10.1016/j.electacta.2015.05.170
The specific and unique amorphous nickel hydroxide nanostructures were synthesized via a simple and straightforward electrochemical way. By simply tuning the soft templates and applying a suitable current density, a specific and unique microstructure is obtained. The diameter of the Ni(OH)2 nano-sphere is greatly influenced by the current density, the sample obtained at 1 mA•cm−2 is about 200 nm while the size of that assembled at 6 mA•cm−2 is less than 20 nm. However, the Ni(OH)2 film prepared at the current density of 2 mA•cm−2 showed the best electrochemical performance for the highly porous surface morphology which contributed to the uniform morphology obtained at this current density. The maximum specific capacitance can be achieved as high as 1460F•g−1 in 2 M NaOH at the scan rate of 2mV•s−1. Such impressive electrochemical properties can be ascribed to the highly porous microstructures and disorder of the amorphous phase which was considered for the better accommodation of repeated volume changes associated with doping-undoping process. The high specific capacitance and remarkable rate capability of amorphous transition metal oxides nanostructures show broad prospect for potential applications in energy conversion and storage devices.
Co-reporter:Wei Wang, Shubo Wang, Handong Jiao, Pan Zhan and Shuqiang Jiao  
Physical Chemistry Chemical Physics 2015 vol. 17(Issue 6) pp:4551-4557
Publication Date(Web):06 Jan 2015
DOI:10.1039/C4CP05764C
Due to their low cost, high abundance and eco-friendly features, Na-ion batteries are becoming alternative choices for rechargeable batteries, especially in large scale applications. Generally, the well-crystallized materials have many advantages over amorphous materials, such as long cycle life, high rate performance and other electrochemical properties. However, the amorphous FePO4 we report here exhibits outstanding cycling stability and rate performance which are derived from its amorphous nature and wafer-like porous morphology. A comparative study of amorphous and crystalline FePO4 has been carried out as cathode materials for Na-ion batteries. The present study not only reports a synthetic method which is facile, inexpensive, and scalable for mass production, but it also motivates further exploration of other amorphous materials for Na-ion batteries.
Co-reporter:Handong Jiao, Junxiang Wang, Long Zhang, Ke Zhang and Shuqiang Jiao  
RSC Advances 2015 vol. 5(Issue 76) pp:62235-62240
Publication Date(Web):09 Jul 2015
DOI:10.1039/C5RA08909C
The electrochemical behavior of titanium ions at a liquid tin cathode has been investigated by cyclic voltammetry and square wave voltammetry in a NaCl–KCl melt at 1023 K. The results show that the deposition potentials of alkali metals and titanium at liquid tin are more positive than those at a solid tungsten cathode. Meanwhile, the results prove that titanium(III) ions can be reduced at liquid tin with a one-step reduction, Ti3+ + 3e = Ti, which is a quasi-reversible process with diffusion-controlled mass transfer. The diffusion coefficient of titanium(III) ions is 1.05 × 10−5 cm2 s−1. Additionally, galvanostatic electrolysis has been carried out to clarify the effect of the current density on the cathodic products. The result demonstrates that a greater depth of titanium will be diffused into the liquid tin cathode during electrolysis with a lower current density.
Co-reporter:Jianbang Ge, Shuai Wang, Feng Zhang, Long Zhang, Handong Jiao, Hongmin Zhu, Shuqiang Jiao
Applied Surface Science 2015 Volume 347() pp:401-405
Publication Date(Web):30 August 2015
DOI:10.1016/j.apsusc.2015.04.119

Highlights

The electrodeposition of carbon films with a Mo2C interlayer.

Carbon diffusion engenders the formation of Mo2C interlayer.

The Mo2C interlayer has a good adhesion.

Co-reporter:Jianbang Ge;Liwen Hu;Wei Wang;Hong Jiao ;Dr. Shuqiang Jiao
ChemElectroChem 2015 Volume 2( Issue 2) pp:224-230
Publication Date(Web):
DOI:10.1002/celc.201402297

Abstract

The capture and electrochemical conversion of CO2 in molten LiCl–Li2CO3 salt is proposed. By using an inert platinum anode and a tungsten cathode, the CO32− could be easily converted into carbon and oxygen gas, as well as O2−. The released O2− was responsible for the further capture of CO2. Also, CO2 could be effectively absorbed in such chloride melts with a low content of oxygen ion dissolved. In addition, the produced carbon displayed good performance as a negative electrode material for Li-ion batteries, suggesting that the process is an environmentally friendly way to convert CO2 into energy-storage materials.

Co-reporter:Jianbang Ge;Liwen Hu;Wei Wang;Hong Jiao ;Dr. Shuqiang Jiao
ChemElectroChem 2015 Volume 2( Issue 2) pp:
Publication Date(Web):
DOI:10.1002/celc.201402178
Co-reporter:Wei Wang, Liwen Hu, Jianbang Ge, Zongqian Hu, Haobo Sun, He Sun, Haiqiang Zhang, Hongmin Zhu, and Shuqiang Jiao
Chemistry of Materials 2014 Volume 26(Issue 12) pp:3721
Publication Date(Web):June 2, 2014
DOI:10.1021/cm501122u
With the growing demands for large-scale applications, rechargeable batteries with cost-effective and environmental-friendly characteristics have gained much attention in recent years. However, some practical challenges still exist in getting ideal electrode materials. In this work, three-dimensional FeWO4/graphene mesoporous composites with incredibly tiny nanospheres of 5–15 nm in diameter have been synthesized by an in situ self-assembled hydrothermal route. First-principles density functional theory has been used to theoretically investigate the crystal structure change and the insertion/extraction mechanism of Li and Na ions. Unlike most graphene-coated materials, which suffer the restacking of graphene layers and experience significant irreversible capacity losses during charge and discharge process, the as-prepared composites have alleviated this issue by incorporating tiny solid nanospheres into the graphene layers to reduce the restacking degree. High capacity and excellent cyclic stability have been achieved for both Li-ion and Na-ion batteries. At the current density of 100 mA g–1, the discharge capacity for Li-ion batteries remains as high as 597 mAh g–1 after 100 cycles. The Na-ion batteries also exhibit good electrochemical performance with a capacity of 377 mAh g–1 at 20 mA g–1 over 50 cycles. The synthetic procedure is simple, cost-effective and scalable for mass production, representing a step further toward the realization of sustainable batteries for efficient stationary energy storage.
Co-reporter:Jiguo Tu, Wei Wang, Liwen Hu, Hongmin Zhu and Shuqiang Jiao  
Journal of Materials Chemistry A 2014 vol. 2(Issue 8) pp:2467-2472
Publication Date(Web):13 Dec 2013
DOI:10.1039/C3TA14719C
A novel SiOxCy film is successfully fabricated by electrodeposition on a carbon paper substrate with vinyl trichlorosilane as the precursor in air. It has been found that the SiOxCy film is evenly and uniformly distributed on the carbon paper. The long-term cycling stability of the SiOxCy film anode is tested at a rate of 1 C for 1000 cycles, showing that the charge capacity decreases from 1919.8 mA h g−1 to 1020.5 mA h g−1 over 1000 cycles, suggesting good long-term cycling stability. The good cycling stability of the SiOxCy film anode is attributed to the ordered structure of the SiOxCy film. Moreover, the interwall space could provide a buffer for Si expansion during the Li insertion/extraction process, thus improving the cycle life of Si anodes.
Co-reporter:Wei Wang, Bo Jiang, Liwen Hu and Shuqiang Jiao  
Journal of Materials Chemistry A 2014 vol. 2(Issue 5) pp:1341-1345
Publication Date(Web):14 Nov 2013
DOI:10.1039/C3TA14310D
A new type of anode material for sodium-ion batteries is proposed which has been synthesized through solid state reaction. The galvanostatic charge/discharge cycling is carried out with a voltage range of 0.01–2.5 V vs. Na+/Na. First-principles calculations are also employed to theoretically investigate the crystal structure change and the insertion–extraction mechanism of Na ions in the NaZr2(PO4)3 structure. The Nasicon material exhibits an excellent reversible charge/discharge capacity under different current densities, which is mainly attributed to the open and strongly bonded NaZr2(PO4)3 structure, allowing the high mobility of the Na ions tunnelling through the PO4–ZrO6 polyhedra chain.
Co-reporter:Haiqiang Zhang, Zongqian Hu, Mao Li, Liwen Hu and Shuqiang Jiao  
Journal of Materials Chemistry A 2014 vol. 2(Issue 40) pp:17024-17030
Publication Date(Web):19 Aug 2014
DOI:10.1039/C4TA03369H
Polythiophene (PTh) was electrochemically polymerized onto the multiwalled carbon nanotube (MWCNT) modified carbon paper by a galvanostatic method in an oil-in-ionic liquid microemulsion (O/IL). The as-prepared PTh/MWCNT composite had an interlaced framework morphology, in which the MWCNTs were uniformly coated by PTh with a thickness of 2–3 nm. The capacitive performance of the as-prepared PTh/MWCNT composite was tested in 1 mol L−1 Na2SO4 solution. The results showed that the composite film had a favorable capacitance with a high electron transfer rate and low resistance. The highest specific capacitance could be achieved as high as 216 F g−1 with the charge loading of 300 mC at a current density of 1 A g−1. The PTh/MWCNT composite had a good cycle stability with a low fading rate of specific capacitance after 500 cycles. The results demonstrated the feasibility of the as-prepared PTh/MWCNT composite to be used as an electrode material for supercapacitors.
Co-reporter:He Sun, Haobo Sun, Wei Wang, Handong Jiao and Shuqiang Jiao  
RSC Advances 2014 vol. 4(Issue 81) pp:42991-42995
Publication Date(Web):28 Aug 2014
DOI:10.1039/C4RA07531E
Insoluble Prussian blue (IPB), Fe4[Fe(CN)6]3, is synthesized at room temperature and found to achieve a relatively high storage capacity of 146 mA h g−1 (at a 20 mA g−1 rate) as the cathode material for Na-ion batteries with high potential plateaus. XRD, SEM and TEM are employed to characterize the morphology and microstructure of the as-synthesized IPB. First-principles calculation is introduced to study the electrochemical mechanism. Generally, the environmental friendliness and low cost of the material make it possible to be used for large-scale electric storage applications.
Co-reporter:Jiguo Tu, Yan Yuan, Handong Jiao and Shuqiang Jiao  
RSC Advances 2014 vol. 4(Issue 31) pp:16380-16384
Publication Date(Web):18 Feb 2014
DOI:10.1039/C4RA00592A
Cu2O–Cu was successfully electrodeposited onto a carbon paper substrate through a potentiostatic procedure with a three-electrode configuration. The results demonstrate that the Cu2O–Cu, electrodeposited at a potential of −0.4 V, evenly and uniformly grows on the carbon paper and displays octahedron shaped nanoparticles with an average edge length of 100 nm. Moreover, the photocurrent density of Cu2O–Cu electrodeposited at a potential of −0.4 V can reach up to 1.2 mA cm−2. In this Cu2O–Cu, the interface between the Cu2O and Cu is suggested as the location of photoinduced electron–hole pair separation, and thus it hinders the rapid surface and bulk recombination of the photoinduced electron–hole pairs. Consequently, the photogenerated electrons can be easily transferred through the Cu metal .
Co-reporter:Liwen Hu, Zongqian Hu, Chang Liu, Zhijing Yu, Xiangyu Cao, Yang Han and Shuqiang Jiao  
RSC Advances 2014 vol. 4(Issue 46) pp:24103-24109
Publication Date(Web):15 May 2014
DOI:10.1039/C4RA02305F
Electrodeposition of ZnO in a novel electrolyte, namely reverse micelles containing zinc nitrate and dissolved oxygen, has been successfully performed. By simply altering the applied current densities or using different substrates, various morphologies are obtained, from 2D ultrathin nanosheets to 3D hierarchical flower-like morphologies, which are quite different from those obtained in conventional electrolytes. Importantly, the behaviors of the soft colloidal templates have a great influence on the morphologies of the ZnO nanostructures. It can be inferred that the versatile deformation, coalescence and rearrangement of the soft colloidal templates also contribute to the specific surface morphologies. The soft colloidal templates are inclined to coalesce and assemble into larger templates on ITO, whereas deformation into different shapes is observed on carbon paper. In this way, an overall new idea to control the shapes and sizes of the template via electrochemistry is proposed.
Co-reporter:Shubo Wang, Liwen Hu, Yuejiao Hu, Shuqiang Jiao
Materials Chemistry and Physics 2014 Volume 146(Issue 3) pp:289-294
Publication Date(Web):14 August 2014
DOI:10.1016/j.matchemphys.2014.03.025
•A composite of Fe2O3 capped by conductive polyaniline (PANI) was synthesized.•The Fe2O3/PANI composite manifests very large discharge capacities.•The composite anode showed a good cycling performance.A composite of Fe2O3 capped by conductive polyaniline (PANI) was synthesized by a facile two-step method through combining homogeneous Fe2O3 suspension prepared by a hydrothermal method and in-situ polymerization of aniline. As anode material for lithium ion batteries, the Fe2O3/PANI composite manifests very large discharge capacities of 1635 mAh g−1, 1480 mAh g−1 at large currents of 1.0 and 2.0 A g−1 (1C and 2C), respectively, as well as good cycling performance and rate capacity. The enhancement of electrochemical performance is attributed to the improved electrical conductivity and effective ion transportation of the composite electrode, in that, PANI keeps the Fe2O3 nanorods uniformly connected and offers conductive contact between the electrolyte and the active electrode materials.
Co-reporter:Haiqiang Zhang, Liwen Hu, Jiguo Tu, Shuqiang Jiao
Electrochimica Acta 2014 120() pp: 122-127
Publication Date(Web):
DOI:10.1016/j.electacta.2013.12.091
Co-reporter:Shubo Wang;Wei Wang;Pan Zhan ;Dr. Shuqiang Jiao
ChemElectroChem 2014 Volume 1( Issue 10) pp:1636-1639
Publication Date(Web):
DOI:10.1002/celc.201402208

Abstract

Hollow α-Fe2O3 nanospheres are synthesized by a carbon-template method. The open channels and tiny particles present within the hollow nanospheres facilitate the penetration of the electrolyte, efficiently reducing the diffusion length for both Na ions and electrons and tolerating volume expansion and particle pulverization. A high discharge capacity of 837.3 mAh g−1 is obtained and obvious voltage plateaus can be observed during the charge and discharge process.

Co-reporter:Jiguo Tu ; Yan Yuan ; Pan Zhan ; Handong Jiao ; Xindong Wang ; Hongmin Zhu
The Journal of Physical Chemistry C 2014 Volume 118(Issue 14) pp:7357-7362
Publication Date(Web):March 17, 2014
DOI:10.1021/jp5011023
SiO2 nanospheres were prepared according to a straightforward approach and evaluated as an anode material for lithium-ion batteries. The morphologies display that the obtained amorphous SiO2 powder has good uniform nanospheres with an average diameter of 400 nm. The SiO2 anode shows an initial charge capacity of 622.1 mAh g–1, and it still remains at 876.7 mAh g–1 even at a rate of 1 C over 500 cycles, showing a certain degree of increase. It can be considered that the superior performances are attributed to the partial generated Si, Li2O, and Li4SiO4 matrixes acting as a shielding layer, hence improving the lithium storage performance. In short, the discussed results suggest that SiO2 nanosphere is a promising anode material to improve the electrochemical performances for lithium-ion batteries.
Co-reporter:Jian-xun Song;Qiu-yu Wang;Guo-jing Hu
International Journal of Minerals, Metallurgy, and Materials 2014 Volume 21( Issue 7) pp:660-665
Publication Date(Web):2014 July
DOI:10.1007/s12613-014-0955-0
TiClx (x = 2.17) was prepared by using titanium sponge to reduce the concentration of TiCl4 in a NaCl-KCl melt under negative pressure. The as-prepared NaCl-KCl-TiClx melt was employed as the electrolyte, and two parallel crude titanium plates and one high-purity titanium plate were used as the anode and cathode, respectively. A series of electrochemical tests were performed to investigate the influence of electrolytic parameters on the current efficiency and quality of cathodic products. The results indicated that the quality of cathodic products was related to the current efficiency, which is significantly dependent on the current density and the initial concentration of titanium ions. The significance of this study is the attainment of high-purity titanium with a low oxygen content of 30 × 10−6.
Co-reporter:Jungang Hou, Zheng Wang, Chao Yang, Huijie Cheng, Shuqiang Jiao and Hongmin Zhu  
Energy & Environmental Science 2013 vol. 6(Issue 11) pp:3322-3330
Publication Date(Web):15 Aug 2013
DOI:10.1039/C3EE41854E
Ta3N5 nanorod arrays were fabricated by nitridation of fluorine-containing tantalum oxide (F–Ta2O5) nanorod arrays grown in situ on Ta substrates by a one-pot vapour-phase hydrothermal induced self-assembly technique. In this protocol, the in situ generation and the morphology of arrays elaborately adjusted by reaction time, play a vital role in the formation of the F–Ta2O5 nanorod arrays and a highly conductive interlayer between the nanorods and the substrate. Due to the shape anisotropy, ordered hierarchical structure and high surface area, a high photoelectrochemical activity was achieved by the optimum Ta3N5 nanorod photoelectrode with a photocurrent density of 1.22 mA cm−2 under AM 1.5G irradiation at 1.23 V vs. RHE (reversible hydrogen electrode). Furthermore, a higher and more stable photocurrent was demonstrated by combining the highly active Ta3N5 nanorods with stable Co3O4/Co(OH)2 (Co3O4/Co(II)) bilayer catalysts when compared with that demonstrated for Co(II)/Ta3N5 and Co3O4/Ta3N5 photoelectrodes, exhibiting that not only is the onset potential negatively shifted but also the photocurrent and the stability are significantly improved, which is correlated to an order of magnitude reduction in the resistance to charge transfer at the Ta3N5/H2O interface. Specifically, about 92% of the initial stable photocurrent remains after long-term irradiation at 1.23 V vs. RHE. At 1.23 V vs. RHE, the photocurrent density of Co3O4/Co(II)/Ta3N5 arrays reached 3.64 mA cm−2 under AM 1.5G simulated sunlight at 100 mW cm−2, and a maximum IPCE of 39.5% was achieved at 440 nm. This combination of catalytic activity, stability, and conformal decoration makes this a promising approach to improve the photoelectrochemical performance of photoanodes in the general field of energy conversion.
Co-reporter:Liwen Hu, Wei Wang, Jiguo Tu, Jungang Hou, Hongmin Zhu and Shuqiang Jiao  
Journal of Materials Chemistry A 2013 vol. 1(Issue 16) pp:5136-5141
Publication Date(Web):25 Feb 2013
DOI:10.1039/C3TA10569E
Amorphous matrices of three-dimensionally interconnected MnOx/MnOOH nano-spheres were electrochemically assembled onto a carbon substrate by a pulse galvanostatic method (PGM) in a nonionic reverse micelle electrolyte. The synthesized material showed a unique morphology which was attributed to a synergistic effect between the amphiphilic molecule based interface membrane as a soft template and the PGM approach. The transfer of the reactant was remarkably special because of the elusive thermodynamic and kinetic parameters of the interactions at the interface between the two different phases such as the polar phase–interface membrane, interface membrane–nonpolar phase and polar phase–electrode interactions. Further work involved investigations into the potential application of the assembled MnOx/MnOOH films as high performance supercapacitor electrode materials. The capacitive performance of the assembled MnOx/MnOOH was tested in a solution of 0.5 M Na2SO4. The highest specific discharge capacitance of 1659 F g−1 was achieved at a current density of 2 A g−1, and remained as high as 782 F g−1 even at a very large current density of 10 A g−1. The outstanding capacitance properties were ascribed to the ternary oxide composites forming highly porous nanostructures which guaranteed a large specific surface, full utilization of Mn oxides and a small amount of degradation of amorphous MnO2. The results indicate the feasibility of electrochemically synthesizing Mn oxides in unconventional micelle electrolytes, and their successful application in supercapacitors.
Co-reporter:Wei Wang, Chengjun Yu, Zheshuai Lin, Jungang Hou, Hongmin Zhu and Shuqiang Jiao  
Nanoscale 2013 vol. 5(Issue 2) pp:594-599
Publication Date(Web):13 Nov 2012
DOI:10.1039/C2NR32661B
Conventionally, rechargeable batteries with a fast charge–discharge rate, while being able to be implemented in large-scale applications with low prices, are critical for new energy storage systems. In this work, first-principles simulations were employed to theoretically investigate the insertion of sodium into the Na2Ti3O7 structure. The result discovered that the theoretical capacity of Na2Ti3O7 was 311 mA h g−1. Furthermore, a microspheric Na2Ti3O7 material consisting of tiny nanotubes of ca. 8 nm in outside diameter and a few hundred nanometers in length has been synthesized. The galvanostatic charge–discharge measurements, using the as-prepared Na2Ti3O7 nanotubes as a working electrode with a voltage range of 0.01–2.5 V vs. Na+/Na, disclosed that a high capacity was maintained even under an ultrafast charge–discharge rate. At a current density of 354 mA g−1, the discharge capacity was maintained at 108 mA h g−1 over 100 cycles. Even at a very large current density of 3540 mA g−1, the discharge capacity was still 85 mA h g−1. HRTEM analysis and electrochemical tests proved that sodium ions could not only intercalate into the Na2Ti3O7 crystal, but could also be stored in the intracavity of the nanotubes. All of the results disclose that the as-prepared Na2Ti3O7 nanotubes are able to be used as anode materials in large-scale applications for rechargeable sodium-ion batteries at low cost while maintaining excellent performance.
Co-reporter:Wei Wang, Hualing Wang, Shubo Wang, Yuejiao Hu, Qixiang Tian, Shuqiang Jiao
Journal of Power Sources 2013 Volume 228() pp:244-249
Publication Date(Web):15 April 2013
DOI:10.1016/j.jpowsour.2012.11.092
Ruthenium doped nanostructured lithium titanates have been synthesized through a reverse microemulsion method with a subsequent sintering process. The as-prepared powders are characterized by the X-ray diffraction and transmission electron microscope techniques. The results indicate that a solid solution of Li4Ti5 − xRuxO12 is formed when x was less than 0.1. The electrochemical performances of the as-prepared materials are investigated in a potential range from 0.01 to 2.5 V by charge and discharge characterizations. In that, the as-prepared Li4Ti4.95Ru0.05O12 exhibits an excellent electrochemical performance. The specific discharge capacity remains as 131 mAh g−1 over 100 cycles even cycled at a large density of 17,500 mA g−1 (60 C-rate). While the current density decreases to be 875 mA g−1(3 C-rate), the corresponding specific discharge capacity is kept as high as 259 mAh g−1 after 100 cycles.Highlights► Synthesis of Ru doped lithium titanate by a reverse microemulsion method. ► Ru doped lithium titanates had an excellent electrochemical performance. ► Ru doped lithium titanates remained high capacity under a large cycled rate.
Co-reporter:Shubo Wang, Jianbang Ge, Yuejiao Hu, Hongmin Zhu, Shuqiang Jiao
Electrochimica Acta 2013 Volume 87() pp:148-152
Publication Date(Web):1 January 2013
DOI:10.1016/j.electacta.2012.09.044
Electrochemical tests, including anodic polarization, Tafel polarization and electrochemical impedance spectrum (EIS), were used to evaluate the anodic behaviors of a ternary alloy of Ni0.94Si0.04Al0.02 in molten NaOH at 773 K. The results revealed that a conductive passivation layer had formed during electrolysis, which protected the Ni0.94Si0.04Al0.02 substrate from further attacked. An in situ test of anodic gases using a mass spectra indicated that oxygen was emitted from the interface of the Ni0.94Si0.04Al0.02 anode. Meanwhile, the iron sponge can be electrochemically produced when Fe2O3 is used as cathode. The significant result is that the Ni0.94Si0.04Al0.02 alloy is promising as an inert anode in molten NaOH electrolyte for a green metallurgical process.
Co-reporter:Wei Wang, Bo Jiang, Weiyi Xiong, Zhen Wang, Shuqiang Jiao
Electrochimica Acta 2013 Volume 114() pp:198-204
Publication Date(Web):30 December 2013
DOI:10.1016/j.electacta.2013.10.035
A nanoparticle Mg-doped Li4Ti5O12 with a grain size of 20–30 nm has been successfully synthesized through a simple hydrothermal method. The first-principle simulations are employed to theoretically study the crystal structure, unit cell volume, lattice parameters, and band gaps. Galvanostatic charge–discharge tests have been carried out, using the as-prepared Li4Ti5O12 and Mg-doped Li4Ti5O12 as the working electrodes with a voltage range of 0.5–2.5 V vs. Li+/Li. The tests show promising results with high capacity and long term stability. When discharging at 350 mA g−1 (corresponding to a 2 C rate), the discharge capacity remains at 170 mAh g−1 over 100 cycles. As the C-rate rises to an ultrafast charge–discharge rate of 50 C, the discharge capacity can still retain at 115 mAh g−1. The excellent electrochemical performance is due to both the nanomorphology and better conductivity after Mg doping. The results show that the Mg-doped Li4Ti5O12 can act as a fast charge–discharge anode material for high rate lithium-ion batteries (LIBs).
Co-reporter:Jiguo Tu, Zuochao Zhao, Liwen Hu, Shuqiang Jiao, Jungang Hou and Hongmin Zhu  
Physical Chemistry Chemical Physics 2013 vol. 15(Issue 25) pp:10472-10476
Publication Date(Web):03 May 2013
DOI:10.1039/C3CP51394G
A 3D-structured anode material, planting core–shell Si@TiN into an amorphous carbon slag (3D STC), was synthesized via a facile pyrolyzing process in assistance with the low-temperature reduction route in a liquid Na–NH3 system. The as-prepared samples were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, cyclic voltammetry and galvanostatic discharge–charge tests. From morphological analysis, TiN nanoparticles were homogeneously dispersed on the surface of Si to form the Si@TiN core–shell structure, subsequently plating into an amorphous C slag to form the 3D STC composite. The electrochemical capacity of the 3D STC anode was measured at a higher rate of 1 C with the cut-off voltages of 0.01 V and 1.5 V. It was found that the initial charge capacity reached up to 1604.6 mA h g−1. In particular, the reversible charge capacity was as high as 588.7 mA h g−1 over 100 cycles, with a small capacity loss of about 0.63% per cycle, exhibiting the excellent cycle stability of the 3D STC anode at the higher rate of 1 C. Furthermore, the reversible capacity of the 3D STC anode decreased from 2048.8 mA h g−1 to 624.0 mA h g−1 with increasing the current rate from 0.1 C to 2 C, while it was still maintained at 1419.7 mA h g−1 as the current rate returned to 0.1 C. Consequentially, the 3D structure with a continuous conductive path could provide facile lithium insertion/extraction and fast electron transfer, making for the high rate capacity and good cycle stability.
Co-reporter:Jiguo Tu, Liwen Hu, Shuqiang Jiao, Jungang Hou and Hongmin Zhu  
Physical Chemistry Chemical Physics 2013 vol. 15(Issue 42) pp:18549-18554
Publication Date(Web):09 Sep 2013
DOI:10.1039/C3CP52777H
The Si–NC core–shell composite was synthesized by a modified oxidative template assembly route using a facile carbonization process. The images of the obtained Si–NC composites showed that an amorphous NC layer adsorbed stably and tightly on the nano-Si surface with an only several nanometers thickness to the formation of the Si–NC core–shell structure, which was beneficial for the electronic contact of Si nanoparticles. For the Si–NC-700 anode, it could be calculated that the initial charge capacity was 986.2 mA h g−1 at a rate of 0.2 C. And it could still be kept at 764.4 mA h g−1 over 100 cycles, with a little capacity loss of 0.22% per cycle. Moreover, it was concluded that the Si–NC-700 anode could achieve a capacity of 790.8 mA h g−1 for the first cycle, and significantly remain at 778.2 mA h g−1 over 500 cycles at a rate of 0.5 C. These excellent electrochemical performances could probably be due to the N-doping generating the extrinsic defects and the absorption of Li ions, and hence result in a superior long-term cycling stability and rate capability. This suggests that the core–shell Si–NC composite is a promising material for improving the electrochemical performance of lithium-ion anodes.
Co-reporter:Jungang Hou, Chao Yang, Huijie Cheng, Zheng Wang, Shuqiang Jiao and Hongmin Zhu  
Physical Chemistry Chemical Physics 2013 vol. 15(Issue 37) pp:15660-15668
Publication Date(Web):17 Jul 2013
DOI:10.1039/C3CP51857D
Highly efficient hydrogen production can be achieved by three-dimensional (3D) architectures of CdS quantum dots (QDs) incorporated in the porous assembly of marigold-like ZnIn2S4 heterostructures coupled with graphene, leading to an efficient electron transfer between them and the enhancement of the ZnIn2S4 photostability. The as-prepared samples were characterized by X-ray diffraction, electron microscopy, Brunauer–Emmett–Teller analysis, X-ray photoelectron spectroscopy, UV-vis diffuse reflectance absorption spectra, and photoluminescence spectra. Especially, 3 wt% CdS QDs decorated ZnIn2S4 heteroarchitectures showed a high rate of H2-production at 1.9 mmol h−1, more 2.7 times than that of ZnIn2S4. The rate was further increased to 2.7 mmol h−1 with a high quantum efficiency of 56% using the 3 wt% CdS QDs decorated ZnIn2S4 composites coupled with 1 wt% graphene (about 4 times higher than that of the pure ZnIn2S4). Moreover, the CdS QDs/graphene/ZnIn2S4 exhibited strong durability due to the high hydrothermal stability of the flower-like structure and the inhibition of CdS leaching owing to its strong interaction with ZnIn2S4. The excellent photocatalytic performance is ascribed to the enhanced light absorption and the improved separation of photogenerated carriers. This finding highlights the validity of 3D semiconductor heterostructures as effective building blocks for exploring efficient visible-light-active photocatalysts.
Co-reporter:Wei Wang, Chengjun Yu, Yingjun Liu, Jungang Hou, Hongmin Zhu and Shuqiang Jiao  
RSC Advances 2013 vol. 3(Issue 4) pp:1041-1044
Publication Date(Web):21 Nov 2012
DOI:10.1039/C2RA22050D
Single crystalline Na2Ti3O7 rods were prepared through sintering a precursor synthesized in a reverse micelle. Charge/discharge measurements were performed in the potential range 0.01–2.5 V versus Na/Na+ under different C-rates. The tested capacity was maintained at 103 mA h g−1, even after 20 cycles at a rate of 0.1 C. The results exhibited that the as-prepared single crystalline Na2Ti3O7 rods had a very low voltage plateau (around 0.3 V), and were suitable to use as anode materials for sodium-ion batteries.
Co-reporter:Jungang Hou, Zheng Wang, Chao Yang, Weilin Zhou, Shuqiang Jiao, and Hongmin Zhu
The Journal of Physical Chemistry C 2013 Volume 117(Issue 10) pp:5132-5141
Publication Date(Web):February 20, 2013
DOI:10.1021/jp311996r
The hierarchical photocatalysts of Ag–AgCl@Bi20TiO32 composites have been successfully synthesized by anchoring Ag–AgCl nanocrystals on the surfaces of mesoporous single-crystalline metastable Bi20TiO32 nanosheets via a two-stage strategy for excellent visible-light-driven photocatalytic activities in the Z-scheme system. First, the single-crystalline metastable Bi20TiO32 nanosheets with tetragonal structures were prepared via a facile hydrothermal process in assistance with the post-heat-treatment route using benzyl alcohol. Especially, the mesoporous Bi20TiO32 nanosheets showed high photocatalytic activity for the degradation of rhodamine B dye under visible-light irradiation. Then, the as-prepared mesoporous Bi20TiO32 nanosheets were used as a support for loading Ag–AgCl nanocrystals using the deposition–precipitation method and irradiation–reduction process to fabricate the Ag–AgCl@Bi20TiO32 composites. Inspiringly, the hierarchical Ag–AgCl@Bi20TiO32 photocatalyst has the higher photocatalytic performance than Ag–AgCl nanocrystals and mesoporous Bi20TiO32 nanosheets over the degradation of rhodamine B and acid orange 7 dyes, which is attributed to the effective charge transfer from plasmon-excited Ag nanocrystal to Bi20TiO32 for the construction of a Z-scheme visible-light photocatalyst. This work could provide new insights into the fabrication of hierarchically plasmonic photocatalysts with high performance and facilitate their practical application in environmental issues.
Co-reporter:Linlin Zhang, Shubo Wang, Shuqiang Jiao, Kai Huang, Hongmin Zhu
Electrochimica Acta 2012 Volume 75() pp:357-359
Publication Date(Web):30 July 2012
DOI:10.1016/j.electacta.2012.05.013
Titanium oxycarbide (TiCxOy) was successfully prepared by an electro-deoxidation of TiO2/C composite cathode in molten calcium chloride at 900 °C. The composite cathode was prepared by adding an amount of carbon into TiO2 powders. By using X-rays diffraction and scanning electron microscopy, it was found that the presence of carbon resulted in changes in reaction mechanism and accelerated the rate of electrochemical reaction. The results suggested that the electrochemical reduction of TiO2/C composite was the following: firstly titanium dioxide was reduced to TiOn (0 < n < 1) along with the formation of CaTiO3. Then, TiOn (0 < n < 1) reacted with carbon to TiCxOy.A schematic diagram of the electrons transmission during electrolysis of TiO2/C.
Co-reporter:Jungang Hou, Zheng Wang, Shuqiang Jiao and Hongmin Zhu  
CrystEngComm 2012 vol. 14(Issue 18) pp:5923-5928
Publication Date(Web):08 Jun 2012
DOI:10.1039/C2CE25504A
The Bi2O3 quantum dots decorated nitrogen doped Bi3NbO7 nanosheets (Bi2O3/N-Bi3NbO7) were successfully synthesized via a facile in situ hydrothermal process as a straightforward protocol. The peony-like N-Bi3NbO7 hierarchical architectures decorated with surface enrichment of Bi2O3 quantum dots were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectra, UV-vis diffuse reflectance spectrum and photoluminescence spectra. The as-prepared Bi2O3/N-Bi3NbO7 heterostructures exhibited higher photocatalytic activities in the decomposition of model pollutants under visible-light irradiation than N-Bi3NbO7 nanosheets in the absence of any expensive metal components and co-catalysts, which could be attributed to the enhanced light absorbance multiple reflections in the heterostructures, the enhanced photosensitizing effect of the surface enriched Bi2O3 quantum dots and the strong interaction between Bi2O3 and N-Bi3NbO7. Furthermore, the Bi2O3/N-Bi3NbO7 heterostructures exhibited strong durability that may be ascribed to the high hydrothermal stability of the flower-like structure and the inhibition of Bi2O3 leaching owing to its tight chemical bonding with N-Bi3NbO7 nanosheets.
Co-reporter:Jiguo Tu, Wei Wang, Shuqiang Jiao, Jungang Hou, Kai Huang, Hongmin Zhu
Materials Chemistry and Physics 2012 Volume 136(2–3) pp:863-867
Publication Date(Web):15 October 2012
DOI:10.1016/j.matchemphys.2012.08.012
High-efficiency Si@TiN composite anode was synthesized by a homogeneous reduction reaction in the liquid ammonia, then calcinated at 950 °C for 2 h in vacuum. The crystal structure and morphology of the obtained in-situ coated composites were characterized by XRD, FESEM. The results showed that the micron-sized Si particles were almost coated by the TiN nanoparticles with the average size of 50 nm, while the morphology of Si@TiN composite was almost unchanged over 50 discharge–charge cycles. The electrochemical performances of Si@TiN composite anode were studied by galvanostatic discharge–charge tests, cyclic voltammetry (CV) and electrochemical impedance spectrum (EIS). The CV curves showed that the two redox peaks remained stable and were attributed to the alloying/dealloying process of Li with active Si particles. It could be seen from the EIS curves that the charge transfer resistance (Rct) for fresh was larger than that for the 50th cycle, which was mainly because the electrons and Li ions conducted on the electrode surface more difficultly for fresh. The cycle stability of the as-prepared Si@TiN composite anode was investigated, with the result showing that the cycling performance was stable and optimal at a rate of 0.2 C. The initial charge capacity was as high as 3226.99 mAh g−1, which was kept as 467.02 mAh g−1 over 50 cycles.Highlights► Si@TiN composite anode was synthesized in-situ in a liquid ammonia. ► The size of TiN nanoparticles was about 50 nm. ► The initial charge capacity was as high as 3226.99 mAh g−1.
Co-reporter:Wen Chen, Shubo Wang, Jianbang Ge, Shuqiang Jiao, Hongmin Zhu
Intermetallics 2012 Volume 25() pp:66-69
Publication Date(Web):June 2012
DOI:10.1016/j.intermet.2012.02.013
Nb5Si3 intermetallic compound was directly synthesized via an electrodeoxidation process from molten CaCl2 electrolyte. The reaction mechanism was studied by performing a series of quenching investigations, which suggested that the formation of a series of sub oxides and compounds containing calcium and oxygen preceded the formation of Nb5Si3. While Nb2O5 was gradually reduced to its sub oxides, (Nb2O5/NbO2/NbO/Nb), SiO2, on the other hand, got directly reduced to silicon and reacted with Nb to form Nb5Si3.Highlights► Nb5Si3 was directly synthesized via electrodeoxidation in molten CaCl2. ► Nb2O5 was gradually reduced to NbO2, NbO and Nb. ► CaNb2O6 was formed at the initial stage and reduced to CaNb2O4 and Nb. ► The formation of Nb5Si3 impelled the decomposition of SiO2.
Co-reporter:Jungang Hou, Rui Cao, Zheng Wang, Shuqiang Jiao and Hongmin Zhu  
Journal of Materials Chemistry A 2011 vol. 21(Issue 20) pp:7296-7301
Publication Date(Web):08 Apr 2011
DOI:10.1039/C0JM04374E
Single-crystalline chromium doped bismuth titanate (Bi4Ti3−xCrxO12, x = 0.0–0.5) nanosheets with exposed {110} facets have been synthesized via a facile hydrothermal process. The Bi4Ti3−xCrxO12nanosheets possess well-defined tetragonal shapes with landscape dimension of 100–300 nm and thickness of 10–30 nm. The in-plane surfaces of the nanosheets lies on {001}, and the side surfaces are (110) and (10). Extension of the light absorption from the ultraviolet region to the visible-light region arises from the Cr 2p levels confirmed by XPS spectra. The Bi4Ti2.6Cr0.4O12 nanosheets with high stability showed the highest photocatalytic performance of H2 evolution from water under visible-light irradiation. Furthermore, the heterostructures by using the NiOx nanoparticles tightly coupled on the surface of Bi4Ti2.6Cr0.4O12 nanosheets, exhibited an enhanced photocatalytic activity due to the decrease in the recombination rate of the photoinduced electrons and holes, demonstrating that NiOx/Bi4Ti2.6Cr0.4O12 nanosheet is a promising candidate as a visible light photocatalyst.
Co-reporter:Shuqiang Jiao, Jiguo Tu, Changyong Fan, Jungang Hou and Derek J. Fray  
Journal of Materials Chemistry A 2011 vol. 21(Issue 25) pp:9027-9030
Publication Date(Web):16 May 2011
DOI:10.1039/C1JM11064K
A polyaniline (PANI) film was electrochemically polymerized onto an ITO substrate by the pulse galvanostatic method in a reverse micelle electrolyte. The morphology of the as-prepared PANI was investigated by using a scanning electron microscope. An interesting result was that a nano-PANI was observed with a diameter of 100 nm. Further work involves investigating the potential application of the PANI films to a high performance supercapacitor electrode material. The energy density of the PANI was measured in HClO4 solution. The highest energy density of nano-PANI arrays was 116.6 W h kg−1 and kept as high 64.1 W h kg−1 at a large charge–discharge current density (10 A g−1). The cycle stability based on the PANI film electrode was investigated. The result showed that it had a low fading rate of its energy density after 500 cycles.
Co-reporter:Jungang Hou, Shuqiang Jiao, Hongmin Zhu and R. V. Kumar  
CrystEngComm 2011 vol. 13(Issue 14) pp:4735-4740
Publication Date(Web):23 May 2011
DOI:10.1039/C1CE05409K
Carbon-modified bismuth titanate (C-Bi12TiO20) nanorods as visible-light-driven photocatalysts were synthesized via a facile hydrothermal process in the presence of glucose followed by the calcinations in Ar gas at 500 °C. The morphology, crystallinity of Bi12TiO20, and the nature of carbon in the composites obtained with different glucose amounts were characterized. Electron microscopy results, light absorption of C-Bi12TiO20 at wavelengths longer than 485 nm and X-ray photoelectron spectra clearly confirmed the carbon modification. Further results indicated that glucose did not affect the final crystalline structure or the band gap of Bi12TiO20, but it had great influence on the photocatalytic activity of Bi12TiO20 towards rhodamine-B (RhB) degradation. It was found that the appropriate amount of carbon can significantly facilitate the separation of photogenerated electron-holes and enhance the photocatalytic degradation efficiency. Especially, the C-Bi12TiO20 photocatalyst using 0.05 g glucose as carbon source can totally decompose RhB after 120 min irradiation. All results demonstrated that this work provides an alternate way to improve the photoactivity of Bi12TiO20 nanomaterial that is promising as a visible-light-driven photocatalyst.
Co-reporter:Jungang Hou, Zheng Wang, Rui Cao, Shuqiang Jiao and Hongmin Zhu  
Dalton Transactions 2011 vol. 40(Issue 16) pp:4038-4041
Publication Date(Web):09 Mar 2011
DOI:10.1039/C0DT01847C
TaON modified by polyaniline (PANI), was prepared through a facile chemisorption process. PANI-modified TaON composites with good stabilities exhibit significantly higher photocatalytic activities than that of neat TaON on degradation of RhB under visible light irradiation, which may result from an enhancement of electron–hole separation between PANI and TaON.
Co-reporter:Jiguo Tu, Jungang Hou, Wei Wang, Shuqiang Jiao, Hongmin Zhu
Synthetic Metals 2011 Volume 161(13–14) pp:1255-1258
Publication Date(Web):July 2011
DOI:10.1016/j.synthmet.2011.04.019
Nano-sized polyaniline (PANI) films were electrochemically deposited onto an ITO substrate by a pulse galvanostatic method (PGM) in an aqueous solution. The morphology of the as-prepared PANI film was characterized using a field emission scanning electron microscope (FESEM). It was observed that the as-prepared PANI films were highly porous, and showed a nano-sized rod-like or coralline-like morphology depending on the charge loading performed in the electropolymerization process. Furthermore, the PANI films were electrochemically measured by the galvanostatic charge–discharge (GCD), cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) tests in 1 mol L−1 HClO4 solution. The results showed that such PANI films had a favorable electrochemical activity and an excellent capacitance. The rod-like PANI film prepared with the charge loading of 1000 mC showed the highest discharge capacitance of 569.1 F g−1 at a low current density of 1 A g−1. The discharge capacitance retained 97.7% after 1000 cycles at a large current density of 10 A g−1.Highlights► Porous nanorod polyaniline films were electrochemically polymerized. ► The highest specific discharge capacitance was 569.1 F g−1. ► The discharge capacitance retained 97.7% over 1000 cycles.
Co-reporter:Jungang Hou;Hongmin Zhu;R. V. Kumar
Journal of Nanoparticle Research 2011 Volume 13( Issue 10) pp:
Publication Date(Web):2011 October
DOI:10.1007/s11051-011-0545-2
Highly crystalline bismuth titanate (Bi12TiO20, BiT) nanorods, as visible-light photocatalysts were prepared by a template-free hydrothermal process. The as-prepared BiT nanorods fabricated in high yields by simply manipulating pH values in the absence of any capping agent, were characterized by a number of techniques, such as XRD, SEM, TEM, HRTEM, BET, and UV–Vis spectrum. In this case, hydroxide ions seem to play a pivotal role in controlling the formation of seeds and the growth of the BiT nanorods. Based on the structural analysis of nanocrystals obtained at different pH values, we proposed a plausible mechanism to account for the formation of the tunable morphologies. Most importantly, the BiT nanorods with good stability exhibited higher photocatalytic activities in the degradation of Rhodamine B under visible light irradiation (λ ≥ 420 nm) than the commercial P25 TiO2 and bulk BiT powders, demonstrating that Bi12TiO20 is a promising candidate as a visible-light photocatalyst.
Co-reporter:Shuqiang Jiao, Linlin Zhang, Hongmin Zhu, Derek J. Fray
Electrochimica Acta 2010 Volume 55(Issue 23) pp:7016-7020
Publication Date(Web):30 September 2010
DOI:10.1016/j.electacta.2010.06.033
NiTi shape memory alloys (SMA) with equiatomic composition of Ni and Ti were prepared by electro-deoxidation, in molten calcium chloride, at 950 °C. Constant voltage electro-deoxidation was conducted using a NiTiO3 cathode, and either a carbon anode or a novel CaRuO3/CaTiO3 composite inert anode. Both anode materials successfully allowed NiTi shape memory alloy to be obtained. The primary difference is that molecular oxygen was produced on the inert anode, instead of environmentally undesired CO2 greenhouse gases on the carbon anode. Indeed, it was found that carbon could successfully be substituted with conductive calcium titanate–calcium ruthenate composites for electro-deoxidation. Furthermore, DSC was used to analyze the phase transformation of NiTi shape memory alloys, with results revealing the existence of reversible martensite–austenite phase transformations during the cooling and heating process.
Co-reporter:Wei Wang, Bo Jiang, Liwen Hu, Zheshuai Lin, Jungang Hou, Shuqiang Jiao
Journal of Power Sources (15 March 2014) Volume 250() pp:
Publication Date(Web):15 March 2014
DOI:10.1016/j.jpowsour.2013.11.016
•The single crystalline VO2 nanosheets have been synthesized.•The reaction during charge/discharge can happen between Na0.3VO2 and NaVO2.•The synthesized material can retain outstanding rate ability.In recent years, with the growing demands for large-scale applications of rechargeable batteries, the eco-friendly sodium-ion batteries with low price and high charge–discharge rates have attracted much attention. In this work, using a simple hydrothermal process, we successfully synthesize single crystalline VO2 parallel ultrathin nanosheets for the cathode material in sodium-ion batteries. Combined the XRD, XPS, electrochemical measurements with the first-principles simulations, the charge–discharge performance and the mechanism of Na insertion and extraction into/from the VO2 structure have systematically studied. The results reveal that the NaxVO2 products possess semiconductor properties and the interlayer distance almost keeps constant during charge and discharge process, which is beneficial to the transmission of Na ions. The charge and discharge process occurs between Na0.3VO2 and NaVO2. Even at a large current density of 500 mA g−1, the discharge capacity can still keep at 108 mAh g−1. As a cathode material for sodium-ion batteries, the results are outstanding and provide a possibility of large-scale applications for rechargeable sodium-ion batteries.
Co-reporter:Haobo Sun, Wei Wang, Zhijing Yu, Yan Yuan, Shuai Wang and Shuqiang Jiao
Chemical Communications 2015 - vol. 51(Issue 59) pp:NaN11895-11895
Publication Date(Web):2015/06/16
DOI:10.1039/C5CC00542F
A new kind of Al-ion battery with carbon paper as the cathode, high-purity Al foil as the anode and ionic liquid as the electrolyte is proposed in this work. The significance of the presented battery is going to be an extremely high average voltage plateau of ca. 1.8 V vs. Al3+/Al.
Co-reporter:Wei Wang, Bo Jiang, Liwen Hu and Shuqiang Jiao
Journal of Materials Chemistry A 2014 - vol. 2(Issue 5) pp:NaN1345-1345
Publication Date(Web):2013/11/14
DOI:10.1039/C3TA14310D
A new type of anode material for sodium-ion batteries is proposed which has been synthesized through solid state reaction. The galvanostatic charge/discharge cycling is carried out with a voltage range of 0.01–2.5 V vs. Na+/Na. First-principles calculations are also employed to theoretically investigate the crystal structure change and the insertion–extraction mechanism of Na ions in the NaZr2(PO4)3 structure. The Nasicon material exhibits an excellent reversible charge/discharge capacity under different current densities, which is mainly attributed to the open and strongly bonded NaZr2(PO4)3 structure, allowing the high mobility of the Na ions tunnelling through the PO4–ZrO6 polyhedra chain.
Co-reporter:Jungang Hou, Rui Cao, Zheng Wang, Shuqiang Jiao and Hongmin Zhu
Journal of Materials Chemistry A 2011 - vol. 21(Issue 20) pp:NaN7301-7301
Publication Date(Web):2011/04/08
DOI:10.1039/C0JM04374E
Single-crystalline chromium doped bismuth titanate (Bi4Ti3−xCrxO12, x = 0.0–0.5) nanosheets with exposed {110} facets have been synthesized via a facile hydrothermal process. The Bi4Ti3−xCrxO12nanosheets possess well-defined tetragonal shapes with landscape dimension of 100–300 nm and thickness of 10–30 nm. The in-plane surfaces of the nanosheets lies on {001}, and the side surfaces are (110) and (10). Extension of the light absorption from the ultraviolet region to the visible-light region arises from the Cr 2p levels confirmed by XPS spectra. The Bi4Ti2.6Cr0.4O12 nanosheets with high stability showed the highest photocatalytic performance of H2 evolution from water under visible-light irradiation. Furthermore, the heterostructures by using the NiOx nanoparticles tightly coupled on the surface of Bi4Ti2.6Cr0.4O12 nanosheets, exhibited an enhanced photocatalytic activity due to the decrease in the recombination rate of the photoinduced electrons and holes, demonstrating that NiOx/Bi4Ti2.6Cr0.4O12 nanosheet is a promising candidate as a visible light photocatalyst.
Co-reporter:Zhijing Yu, Zepeng Kang, Zongqian Hu, Jianhong Lu, Zhigang Zhou and Shuqiang Jiao
Chemical Communications 2016 - vol. 52(Issue 68) pp:NaN10430-10430
Publication Date(Web):2016/07/26
DOI:10.1039/C6CC05974K
Hexagonal NiS nanobelts served as novel cathode materials for rechargeable Al-ion batteries based on an AlCl3/[EMIm]Cl ionic liquid electrolyte system. The nano-banded structure of the materials can facilitate the electrolyte immersion and enhance Al3+ diffusion. The hexagonal NiS nanobelt based cathodes exhibit high storage capacity, good cyclability and low overpotential.
Co-reporter:Haiqiang Zhang, Zongqian Hu, Mao Li, Liwen Hu and Shuqiang Jiao
Journal of Materials Chemistry A 2014 - vol. 2(Issue 40) pp:NaN17030-17030
Publication Date(Web):2014/08/19
DOI:10.1039/C4TA03369H
Polythiophene (PTh) was electrochemically polymerized onto the multiwalled carbon nanotube (MWCNT) modified carbon paper by a galvanostatic method in an oil-in-ionic liquid microemulsion (O/IL). The as-prepared PTh/MWCNT composite had an interlaced framework morphology, in which the MWCNTs were uniformly coated by PTh with a thickness of 2–3 nm. The capacitive performance of the as-prepared PTh/MWCNT composite was tested in 1 mol L−1 Na2SO4 solution. The results showed that the composite film had a favorable capacitance with a high electron transfer rate and low resistance. The highest specific capacitance could be achieved as high as 216 F g−1 with the charge loading of 300 mC at a current density of 1 A g−1. The PTh/MWCNT composite had a good cycle stability with a low fading rate of specific capacitance after 500 cycles. The results demonstrated the feasibility of the as-prepared PTh/MWCNT composite to be used as an electrode material for supercapacitors.
Co-reporter:Handong Jiao, Chen Wang, Jiguo Tu, Donghua Tian and Shuqiang Jiao
Chemical Communications 2017 - vol. 53(Issue 15) pp:NaN2334-2334
Publication Date(Web):2017/01/23
DOI:10.1039/C6CC09825H
A new Al-ion battery based on an affordable and nontoxic liquid electrolyte made from molten AlCl3/urea was assembled. As the cathode material, natural graphite shows two well-defined discharge voltage plateaus at about 1.9 and 1.5 V with a high specific capacity of 93 mA h g−1 and excellent coulombic efficiency (>99%). The attractive capacity (about 78 mA h g−1) is retained even at a high current density of 1000 mA g−1. Moreover, no faster fading in capacity is observed after 500 cycles. This electrolyte could provide a new system for Al ion batteries, which can be used for large scale energy storage, owing to its cost advantages, high-rate capability and durability.
Co-reporter:Liwen Hu, Yang Song, Jianbang Ge, Jun Zhu, Zhenchao Han and Shuqiang Jiao
Journal of Materials Chemistry A 2017 - vol. 5(Issue 13) pp:NaN6225-6225
Publication Date(Web):2017/02/28
DOI:10.1039/C7TA00258K
As part of the efforts to address global climate change, the identification of methods for the capture of carbon dioxide and its selective electrochemical conversion into value-added carbonaceous materials in molten salt electrolytes is a research topic of scientific and technological significance. In most cases, metal electrodes such as nickel and stainless steel are used as the cathode to investigate the nucleation and growth of a variety of carbon nanostructures. In this study, the electrochemical deposition of carbon nanotubes (CNTs) and carbon microstructures was performed in molten CaCl2–NaCl–CaO using glassy carbon and graphite rod as the cathode and RuO2–TiO2 as the anode. The capture formula was established and the capture coefficient was defined and calculated to be 1.8 s−1. Cyclic voltammetry, constant voltage electrolysis, as well as on-line outlet gas analysis were conducted to investigate the electrode reactions, and the results indicated that the captured CO2 can be electrochemically converted to carbon and environmentally-friendly oxygen as the only by-product. SEM and TEM images showed that quasi-spherical and nanotubular carbon were deposited on the graphite and glassy carbon cathodes at 750 °C. However, by regulating the temperature, quasi-spheres and nanosheets were observed at the glassy carbon cathode.
Co-reporter:Yang Song, Shuqiang Jiao, Jiguo Tu, Junxiang Wang, Yingjun Liu, Handong Jiao, Xuhui Mao, Zhancheng Guo and Derek J. Fray
Journal of Materials Chemistry A 2017 - vol. 5(Issue 3) pp:NaN1291-1291
Publication Date(Web):2016/12/06
DOI:10.1039/C6TA09829K
Affordable and scalable energy storage systems are necessary to mitigate the output fluctuation of an electrical power grid integrating intermittent renewable energy sources. Conventional battery technologies are unable to meet the demanding low-cost and long-life span requirements of a grid-scale application, although some of them demonstrated impressive high energy density and capacity. More recently, the prototype of an Al-ion battery has been developed using cheap electrode materials (Al and graphite) in an organic room-temperature ionic liquid electrolyte. Here we implement a different Al-ion battery in an inorganic molten salt electrolyte, which contains only an extremely low-cost and nonflammable sodium chloroaluminate melt working at 120 °C. Due to the superior ionic conductivity of the melt electrolyte and the enhanced Al-ion interaction/deintercalation dynamics at an elevated temperature of 120 °C, the battery delivered a discharge capacity of 190 mA h g−1 at a current density of 100 mA g−1 and showed an excellent cyclic performance even at an extremely high current density of 4000 mA g−1: 60 mA h g−1 capacity after 5000 cycles and 43 mA h g−1 capacity after 9000 cycles, with a coulombic efficiency constantly higher than 99%. The low-cost and safe characteristics, as well as the outstanding long-term cycling capability at high current densities allow the scale-up of this brand-new battery for large-scale energy storage applications.
Co-reporter:Jiguo Tu, Liwen Hu, Shuqiang Jiao, Jungang Hou and Hongmin Zhu
Physical Chemistry Chemical Physics 2013 - vol. 15(Issue 42) pp:NaN18554-18554
Publication Date(Web):2013/09/09
DOI:10.1039/C3CP52777H
The Si–NC core–shell composite was synthesized by a modified oxidative template assembly route using a facile carbonization process. The images of the obtained Si–NC composites showed that an amorphous NC layer adsorbed stably and tightly on the nano-Si surface with an only several nanometers thickness to the formation of the Si–NC core–shell structure, which was beneficial for the electronic contact of Si nanoparticles. For the Si–NC-700 anode, it could be calculated that the initial charge capacity was 986.2 mA h g−1 at a rate of 0.2 C. And it could still be kept at 764.4 mA h g−1 over 100 cycles, with a little capacity loss of 0.22% per cycle. Moreover, it was concluded that the Si–NC-700 anode could achieve a capacity of 790.8 mA h g−1 for the first cycle, and significantly remain at 778.2 mA h g−1 over 500 cycles at a rate of 0.5 C. These excellent electrochemical performances could probably be due to the N-doping generating the extrinsic defects and the absorption of Li ions, and hence result in a superior long-term cycling stability and rate capability. This suggests that the core–shell Si–NC composite is a promising material for improving the electrochemical performance of lithium-ion anodes.
Co-reporter:Liwen Hu, Wei Wang, Jiguo Tu, Jungang Hou, Hongmin Zhu and Shuqiang Jiao
Journal of Materials Chemistry A 2013 - vol. 1(Issue 16) pp:NaN5141-5141
Publication Date(Web):2013/02/25
DOI:10.1039/C3TA10569E
Amorphous matrices of three-dimensionally interconnected MnOx/MnOOH nano-spheres were electrochemically assembled onto a carbon substrate by a pulse galvanostatic method (PGM) in a nonionic reverse micelle electrolyte. The synthesized material showed a unique morphology which was attributed to a synergistic effect between the amphiphilic molecule based interface membrane as a soft template and the PGM approach. The transfer of the reactant was remarkably special because of the elusive thermodynamic and kinetic parameters of the interactions at the interface between the two different phases such as the polar phase–interface membrane, interface membrane–nonpolar phase and polar phase–electrode interactions. Further work involved investigations into the potential application of the assembled MnOx/MnOOH films as high performance supercapacitor electrode materials. The capacitive performance of the assembled MnOx/MnOOH was tested in a solution of 0.5 M Na2SO4. The highest specific discharge capacitance of 1659 F g−1 was achieved at a current density of 2 A g−1, and remained as high as 782 F g−1 even at a very large current density of 10 A g−1. The outstanding capacitance properties were ascribed to the ternary oxide composites forming highly porous nanostructures which guaranteed a large specific surface, full utilization of Mn oxides and a small amount of degradation of amorphous MnO2. The results indicate the feasibility of electrochemically synthesizing Mn oxides in unconventional micelle electrolytes, and their successful application in supercapacitors.
Co-reporter:Wei Wang, Shubo Wang, Handong Jiao, Pan Zhan and Shuqiang Jiao
Physical Chemistry Chemical Physics 2015 - vol. 17(Issue 6) pp:NaN4557-4557
Publication Date(Web):2015/01/06
DOI:10.1039/C4CP05764C
Due to their low cost, high abundance and eco-friendly features, Na-ion batteries are becoming alternative choices for rechargeable batteries, especially in large scale applications. Generally, the well-crystallized materials have many advantages over amorphous materials, such as long cycle life, high rate performance and other electrochemical properties. However, the amorphous FePO4 we report here exhibits outstanding cycling stability and rate performance which are derived from its amorphous nature and wafer-like porous morphology. A comparative study of amorphous and crystalline FePO4 has been carried out as cathode materials for Na-ion batteries. The present study not only reports a synthetic method which is facile, inexpensive, and scalable for mass production, but it also motivates further exploration of other amorphous materials for Na-ion batteries.
Co-reporter:Jungang Hou, Zheng Wang, Rui Cao, Shuqiang Jiao and Hongmin Zhu
Dalton Transactions 2011 - vol. 40(Issue 16) pp:NaN4041-4041
Publication Date(Web):2011/03/09
DOI:10.1039/C0DT01847C
TaON modified by polyaniline (PANI), was prepared through a facile chemisorption process. PANI-modified TaON composites with good stabilities exhibit significantly higher photocatalytic activities than that of neat TaON on degradation of RhB under visible light irradiation, which may result from an enhancement of electron–hole separation between PANI and TaON.
Co-reporter:Jungang Hou, Chao Yang, Huijie Cheng, Zheng Wang, Shuqiang Jiao and Hongmin Zhu
Physical Chemistry Chemical Physics 2013 - vol. 15(Issue 37) pp:NaN15668-15668
Publication Date(Web):2013/07/17
DOI:10.1039/C3CP51857D
Highly efficient hydrogen production can be achieved by three-dimensional (3D) architectures of CdS quantum dots (QDs) incorporated in the porous assembly of marigold-like ZnIn2S4 heterostructures coupled with graphene, leading to an efficient electron transfer between them and the enhancement of the ZnIn2S4 photostability. The as-prepared samples were characterized by X-ray diffraction, electron microscopy, Brunauer–Emmett–Teller analysis, X-ray photoelectron spectroscopy, UV-vis diffuse reflectance absorption spectra, and photoluminescence spectra. Especially, 3 wt% CdS QDs decorated ZnIn2S4 heteroarchitectures showed a high rate of H2-production at 1.9 mmol h−1, more 2.7 times than that of ZnIn2S4. The rate was further increased to 2.7 mmol h−1 with a high quantum efficiency of 56% using the 3 wt% CdS QDs decorated ZnIn2S4 composites coupled with 1 wt% graphene (about 4 times higher than that of the pure ZnIn2S4). Moreover, the CdS QDs/graphene/ZnIn2S4 exhibited strong durability due to the high hydrothermal stability of the flower-like structure and the inhibition of CdS leaching owing to its strong interaction with ZnIn2S4. The excellent photocatalytic performance is ascribed to the enhanced light absorption and the improved separation of photogenerated carriers. This finding highlights the validity of 3D semiconductor heterostructures as effective building blocks for exploring efficient visible-light-active photocatalysts.
Co-reporter:Liwen Hu, Yang Song, Jianbang Ge, Jun Zhu and Shuqiang Jiao
Journal of Materials Chemistry A 2015 - vol. 3(Issue 42) pp:NaN21218-21218
Publication Date(Web):2015/09/09
DOI:10.1039/C5TA05127D
Molten CaCl2 is reported to be a potential dopant for reactivation of CaO and enhancement of the cyclic capture ability of CaO. The present work showed that O2− in molten CaCl2–CaO has a strong affinity for CO2 at 850 °C, with resulting formation of carbonates. Using a RuO2·TiO2 inert anode, the formed carbonates were successfully electrochemically split into value-added ultrathin graphite sheets, which look like a kind of graphene, accompanied by evolution of carbon monoxide at the cathode and environmentally friendly by-product oxygen at the anode. The reduction mechanism of CO32− was investigated by cyclic voltammetry and square wave voltammetry. Results demonstrated that there are two steps in electrochemical reduction of CO32−, and the transferred electron numbers calculated for each step are 1.76 and 1.99, respectively. The kind of graphene generated at the cathode may have applications in fields such as energy storage and electronic devices. The molten CaCl2–CaO has potential applications and prospects in large-scale capture of CO2, and electrochemical conversion of CO2 into high value added carbon material such as ultrathin graphite sheets with renewable energy sources.
Co-reporter:Jiguo Tu, Wei Wang, Liwen Hu, Hongmin Zhu and Shuqiang Jiao
Journal of Materials Chemistry A 2014 - vol. 2(Issue 8) pp:NaN2472-2472
Publication Date(Web):2013/12/13
DOI:10.1039/C3TA14719C
A novel SiOxCy film is successfully fabricated by electrodeposition on a carbon paper substrate with vinyl trichlorosilane as the precursor in air. It has been found that the SiOxCy film is evenly and uniformly distributed on the carbon paper. The long-term cycling stability of the SiOxCy film anode is tested at a rate of 1 C for 1000 cycles, showing that the charge capacity decreases from 1919.8 mA h g−1 to 1020.5 mA h g−1 over 1000 cycles, suggesting good long-term cycling stability. The good cycling stability of the SiOxCy film anode is attributed to the ordered structure of the SiOxCy film. Moreover, the interwall space could provide a buffer for Si expansion during the Li insertion/extraction process, thus improving the cycle life of Si anodes.
Co-reporter:Shuai Wang, Wei Wang, Pan Zhan, Yan Yuan, Kailong Jiao, Handong Jiao and Shuqiang Jiao
Journal of Materials Chemistry A 2015 - vol. 3(Issue 32) pp:NaN16534-16534
Publication Date(Web):2015/07/07
DOI:10.1039/C5TA03160E
The synthesis and electrochemical performance derived from NaHTi3O7 have been investigated for use as an anode material for sodium-ion batteries. NaHTi3O7 nanotubes were fabricated by a hydrothermal method. Galvanostatic charge/discharge measurements were performed in a voltage range of 0.01–2.5 V vs. Na+/Na at different current densities, using the as-prepared NaHTi3O7 nanotubes as the working electrode. Typically, the initial discharge and charge capacities of NaHTi3O7 nanotubes were 381.80 mA h g−1 and 242.82 mA h g−1, respectively, at a current density of 20 mA g−1, and still retained a high specific capacity of 105.32 mA h g−1 and 100.65 mA h g−1 after 100 cycles. The electrode also exhibits outstanding rate capability with a reversible capacity as high as 300.95 mA h g−1 and 209.10 mA h g−1 at current densities of 50 mA g−1 and 100 mA g−1, respectively. The excellent electrochemical stability and high specific capacity of these nanostructured materials have been attributed to the three-dimensional flower-like morphology of NaHTi3O7 nanotubes. All of the findings demonstrate that NaHTi3O7 nanotubes have steady cycling performance and environmental and cost friendliness for use in next generation secondary batteries of sodium-ion batteries.
Co-reporter:Shuqiang Jiao, Jiguo Tu, Changyong Fan, Jungang Hou and Derek J. Fray
Journal of Materials Chemistry A 2011 - vol. 21(Issue 25) pp:NaN9030-9030
Publication Date(Web):2011/05/16
DOI:10.1039/C1JM11064K
A polyaniline (PANI) film was electrochemically polymerized onto an ITO substrate by the pulse galvanostatic method in a reverse micelle electrolyte. The morphology of the as-prepared PANI was investigated by using a scanning electron microscope. An interesting result was that a nano-PANI was observed with a diameter of 100 nm. Further work involves investigating the potential application of the PANI films to a high performance supercapacitor electrode material. The energy density of the PANI was measured in HClO4 solution. The highest energy density of nano-PANI arrays was 116.6 W h kg−1 and kept as high 64.1 W h kg−1 at a large charge–discharge current density (10 A g−1). The cycle stability based on the PANI film electrode was investigated. The result showed that it had a low fading rate of its energy density after 500 cycles.
Co-reporter:Jiguo Tu, Zuochao Zhao, Liwen Hu, Shuqiang Jiao, Jungang Hou and Hongmin Zhu
Physical Chemistry Chemical Physics 2013 - vol. 15(Issue 25) pp:NaN10476-10476
Publication Date(Web):2013/05/03
DOI:10.1039/C3CP51394G
A 3D-structured anode material, planting core–shell Si@TiN into an amorphous carbon slag (3D STC), was synthesized via a facile pyrolyzing process in assistance with the low-temperature reduction route in a liquid Na–NH3 system. The as-prepared samples were characterized by X-ray diffraction, field emission scanning electron microscopy, transmission electron microscopy, cyclic voltammetry and galvanostatic discharge–charge tests. From morphological analysis, TiN nanoparticles were homogeneously dispersed on the surface of Si to form the Si@TiN core–shell structure, subsequently plating into an amorphous C slag to form the 3D STC composite. The electrochemical capacity of the 3D STC anode was measured at a higher rate of 1 C with the cut-off voltages of 0.01 V and 1.5 V. It was found that the initial charge capacity reached up to 1604.6 mA h g−1. In particular, the reversible charge capacity was as high as 588.7 mA h g−1 over 100 cycles, with a small capacity loss of about 0.63% per cycle, exhibiting the excellent cycle stability of the 3D STC anode at the higher rate of 1 C. Furthermore, the reversible capacity of the 3D STC anode decreased from 2048.8 mA h g−1 to 624.0 mA h g−1 with increasing the current rate from 0.1 C to 2 C, while it was still maintained at 1419.7 mA h g−1 as the current rate returned to 0.1 C. Consequentially, the 3D structure with a continuous conductive path could provide facile lithium insertion/extraction and fast electron transfer, making for the high rate capacity and good cycle stability.
Calcium, compd. with cobalt (3:1)
Carbon silicon oxide
Potassium ion (1+)
Titanium, chlorooxo-(9CI)
Ferrate(3-),hexakis(cyano-kC)-,copper(2+) (2:3), (OC-6-11)-
Iron tungsten oxide(FeWO4)
Iron tungsten oxide
Iron alloy, Fe,Ni
Sulfuric acid, ammonium iron salt (8CI,9CI)