Co-reporter:Wenpeng Ni, Shimin Liu, Yuqing Fei, Yude He, Xiangyuan Ma, Liujin Lu, and Youquan Deng
ACS Applied Materials & Interfaces May 3, 2017 Volume 9(Issue 17) pp:14749-14749
Publication Date(Web):April 13, 2017
DOI:10.1021/acsami.6b16531
Considering the significant influence of oxygen-containing groups on the surface of carbon involved electrodes, a carbon nanotube (CNT)-based MnO2 composite catalyst was synthesized following a facile method while using polymerized ionic liquids (PIL) as sacrifice agent. Herein, the PIL (polymerized hydrophobic 1-vinyl-3-ethylimidazolium bis ((trifluoromethyl)sulfonyl)imide) wrapped CNTs were prepared. The composite was applied to support MnO2 by the treatment of KMnO4 solution, taking advantage of the reaction between PIL and KMnO4, which excludes or suppresses the oxidation of CNTs, and the as-synthesized material with fewer oxygen-containing groups acted as a cathode catalyst for Li-O2 batteries, directly avoiding the application of binders. The catalyst shows enhanced activity compared to that of the samples without PIL, as verified by the lower overpotential during discharging and charging (0.97 V at the current density of 100 mA g–1). Meanwhile, the performance parameters such as Coulombic efficiency and rate capability were also improved for the Li-O2 battery utilizing this catalyst. Further, the formation of confined Li2O2 particles could be responsible for the reduction of charge potential of Li-O2 batteries due to the synergy effect of the intrinsic catalytic activity of MnO2 and fewer oxygen functional groups on the catalyst surface.Keywords: carbon nanotubes; Li-O2 batteries; manganese dioxide; oxygen-containing groups; polymerized ionic liquids;
Co-reporter:Shiguo Zhang, Jiaheng Zhang, Yan Zhang, and Youquan Deng
Chemical Reviews May 24, 2017 Volume 117(Issue 10) pp:6755-6755
Publication Date(Web):December 29, 2016
DOI:10.1021/acs.chemrev.6b00509
Ionic liquids (ILs) have been widely investigated as novel solvents, electrolytes, and soft functional materials. Nevertheless, the widespread applications of ILs in most cases have been hampered by their liquid state. The confinement of ILs into nanoporous hosts is a simple but versatile strategy to overcome this problem. Nanoconfined ILs constitute a new class of composites with the intrinsic chemistries of ILs and the original functions of solid matrices. The interplay between these two components, particularly the confinement effect and the interactions between ILs and pore walls, further endows ILs with significantly distinct physicochemical properties in the restricted space compared to the corresponding bulk systems. The aim of this article is to provide a comprehensive review of nanoconfined ILs. After a brief introduction of bulk ILs, the synthetic strategies and investigation methods for nanoconfined ILs are documented. The local structure and physicochemical properties of ILs in diverse porous hosts are summarized in the next sections. The final section highlights the potential applications of nanoconfined ILs in diverse fields, including catalysis, gas capture and separation, ionogels, supercapacitors, carbonization, and lubrication. Further research directions and perspectives on this topic are also provided in the conclusion.
Co-reporter:Wenpeng Ni, Shimin Liu, Chao Du, Yuqing Fei, ... Youquan Deng
International Journal of Hydrogen Energy 2017 Volume 42, Issue 30(Volume 42, Issue 30) pp:
Publication Date(Web):27 July 2017
DOI:10.1016/j.ijhydene.2017.06.194
•Co2P and N, P, F-doped mesoporous carbon was synthesized.•The phosphorus sources could affect the morphology and component of the catalysts.•The catalyst prepared by P4444PF6 displays the best activity in all samples.•Zn-air cell with this catalyst exhibit higher discharge potential and power density.There is growing interest in the research of electrocatalysts for oxygen reduction reaction (ORR), which is the key issue for the commercialization of zinc-air (Zn-air) battery. Except precious metal based electrocatalysts, heteroatom-doped carbon materials, as one promising catalyst, also show excellent catalytic activity for ORR. In this work, cobalt phosphide (Co2P) and nitrogen, fluorine and phosphorus co-doped mesoporous carbon is synthesized in one step by a phosphorus-containing ionic liquids assisted route. Owing to the synergy effect of Co2P and functionalized mesoporous carbon, the catalyst exhibits a high half-wave potential of 0.86 V (vs reversible hydrogen electrode) which is about 30 mV positive than commercial Pt/C, coupled with outstanding stability. At last, the discharge potential of the primary zinc-air battery based on this catalyst is 1.1 V at a constant current density of 50 mA cm−2 (150 mV higher than Pt/C electrode) while the capacity is about 800 mAh g−1Zn. At the same time, the superior power density is also realized for the zinc-air battery using this catalyst (180 mW cm−2).Download high-res image (129KB)Download full-size image
Co-reporter:Jianhao Gong;Fulong Yang;Qunfeng Shao;Xiaodong He;Xiaoping Zhang;Shimin Liu;Liyun Tang
RSC Advances (2011-Present) 2017 vol. 7(Issue 67) pp:41980-41988
Publication Date(Web):2017/08/29
DOI:10.1039/C7RA06709G
Here, for the first time, we propose a simple strategy to realize an ultra-wideband metamaterial absorber by using room temperature ionic liquids (ILs) which are a new class of organic salts containing purely anions and cations. At first, the microwave loss characteristics of methylimidazolium ILs were investigated. The results reveal that these ILs have large ionic conductivities and dielectric loss factors which means high conductive loss and dielectric loss of microwaves can both be caused, and the IL with a shorter carbon chain on cation has potential to produce a higher absorption. When the IL [EMIm][N(CN)2] is properly arranged into periodic cylinders supported by a 3D-printed dielectric bracket, impedance matching can be enhanced in a wide band, and a strong absorption of microwave above 90% can be achieved within the whole frequency range of 8.4–29.0 GHz, which was verified in simulations and experiments. In addition, the IL-based metamaterial absorber can work efficiently at arbitrary polarization angles and wide incident angles from 0° to 45°. Mechanism investigations show that the perfect absorption in ILs-based MMAs is mainly originated from the loss of dielectric polarization and induced ionic currents in ILs. Distinct from metamaterial absorbers based on water or other liquids, such IL-based metamaterial absorber can not only broaden the absorption bandwidth significantly, but also have potential application in a wider temperature range because of the exceedingly high thermal stabilities of ILs.
Co-reporter:Xiaodong He;Wenbin Qiang;Chao Du;Qunfeng Shao;Xiaoping Zhang
Journal of Materials Chemistry A 2017 vol. 5(Issue 36) pp:19159-19167
Publication Date(Web):2017/09/19
DOI:10.1039/C7TA05890J
In this study, we develop an innovative low voltage reversible electrowetting of water droplet based on perfluorinated silane-modified slippery lubricant-infused porous surface (SLIPS) that is impregnated by silicone oil. The electrowetting properties of SLIPS modified with and without 1H,1H,2H,2H-perfluorooctyltrichlorosilane (PFOTS) are investigated initially. After modifying the lubricated PTFE membrane with PFOTS, the driving voltage of electrowetting decreases sharply; the threshold voltage is only 5 V, which exhibits an immediate 15-fold decrease compared to that of the unmodified SLIPS. Subsequently, the electrowetting reversibility based on SLIPS modified with different concentrations of PFOTS solution is studied. Our results show that the initial contact angle increases with an increase in the concentration of PFOTS solution, but the electrowetting reversibility has an obvious depravation. The optimal concentration is about 0.03 wt%, in which the electrowetting hysteresis is less than 5°, and a large modulation can be achieved in the contact angle ranging from 107° to 60° with 60 V driving voltage in ambient air. On the basis of surface topography characterization, this low voltage electrowetting is attributed to the contact interface transformation from liquid–oil interface to the combination of liquid–oil and liquid–PFOTS interface. Therefore, the surfaces maintain low surface energy property of PFOTS and retain SLIPS property. In addition, a marked asymmetric contact angle variation with respect to voltage polarity on SLIPS modified with PFOTS is observed for the first time; the low voltage electrowetting occurs at positive voltage but does not occur at negative voltage. Our study provides a new pathway to achieve low voltage electrowetting without decreasing the thickness of the dielectric layer or increasing the dielectric constant.
Co-reporter:Yan Long;Shimin Liu;Yuqing Fei;Qinghe Li
Science China Chemistry 2017 Volume 60( Issue 7) pp:964-969
Publication Date(Web):26 April 2017
DOI:10.1007/s11426-016-9002-x
Nano CuO/ZSM-5 zeolite was prepared and used as a catalyst for dehydration of 1,4-butanediol (BDO) to tetrahydrofuran (THF) in liquid-phase. It was found that the 4.6 wt% CuO/ZSM-5 displayed good catalytic performance, and nearly 100% of BDO conversion and more than 99% of THF selectivity could be achieved by a rotary evaporator reactor at 170 °C under the atmospheric pressure. With such mild reaction conditions, 2400 g BDO could be converted to THF over 1 g catalyst under semi-continuous operation. Characterizations with X-ray diffraction (XRD), temperature-programmed reduction (TPR), NH3-temperature programmed desorption (TPD), X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM) and Brunauer-Emmett-Teller (BET) over fresh and used 4.6 wt% CuO/ZSM-5 were conducted. Based on the results of the characterization and catalytic performance of 4.6 wt% CuO/ZSM-5, it can be conjectured that the formed 1–3 nm CuO nanoparticles, suitable acidity of the catalyst due to the synergic interaction of CuO and ZSM-5 support promoted the dehydration of BDO to THF.
Co-reporter:Peixue Wang;Shimin Liu
Chinese Journal of Chemistry 2017 Volume 35(Issue 6) pp:821-835
Publication Date(Web):2017/06/01
DOI:10.1002/cjoc.201600745
Currently, industrial production of isocyanates, or diisocyanates in particular, has been exclusively based on phosgene processes. Phosgene is extremely toxic and large amounts of corrosive HCl are produced as a side product. In the view of environment protection and society safety, development of non-phosgene processes for isocyanates production will be highly desired, and this should be one of the most important missions for green chemistry and catalysis. In this review, efforts for development of non-phosgene method for syntheses of isocyanates, i.e., catalytic syntheses of N-substituted carbamates from nitro- or amino-compounds with CO, dimethyl carbonate (DMC), urea and even CO2 etc. as carbonyl sources, then thermal cracking of N-substituted carbamates to afford corresponding isocyanates, are summarized, and a brief prospect for non-phosgene syntheses of isocyanates is also addressed.
Co-reporter:Shiguo Zhang, Qinghua Zhang, Yan Zhang, Zhengjian Chen, Masayoshi Watanabe, Youquan Deng
Progress in Materials Science 2016 Volume 77() pp:80-124
Publication Date(Web):April 2016
DOI:10.1016/j.pmatsci.2015.10.001
Instead of being seen as alternative solvents and electrolytes for organic reactions, catalysis, separation, electrochemistry, and so on, ionic liquids (ILs) consisting of discrete cations and anions have recently emerged as versatile building blocks for advanced functional materials. A number of functional ILs and IL-containing composite materials have been realized by either chemical modification (covalent functionalization or ion-exchange metathesis) or physical integration of ILs and traditional materials. The unique structure and behavior of ILs as a platform not only provides additional opportunities to adjust the physicochemical properties of these ionic materials for task-specific applications, but also offers other attractive features such as intrinsic ionic conductivity and high thermal, chemical, and electrochemical stability. These soft materials combine the favorable features of ILs and the original chemistries of the functional groups or materials; some even possess unexpected functions resulting from synergetic interaction between these two components. Materialization of ILs is truly a novel, promising research direction for both IL chemistry and materials science. In this article, we review recent advances in IL-based functional materials, focusing on smart and sensitive materials, optical materials, energetic materials, and IL/carbon hybrid materials.
Co-reporter:Wenpeng Ni, Shimin Liu, Yuqing Fei, Yude He, Xiangyuan Ma, Liujin Lu and Youquan Deng
Journal of Materials Chemistry A 2016 vol. 4(Issue 20) pp:7746-7753
Publication Date(Web):14 Apr 2016
DOI:10.1039/C6TA01222A
The catalytic activity of a cathode material plays a vital role in determining the electrochemical performance of Li–O2 batteries. Herein, N-doped mesoporous carbon-supported CoO@Co nanoparticles are prepared in situ using the ionic liquid (IL) 1-butyl-3-methylimidazolium tetrachlorocobalt ([BMIm]2[CoCl4]) as the precursor with silica as the hard template. The material was characterized by TGA, BET, XRD, TEM, XPS, and H2-TPR. After exposure to air, the species on the surface of the Co is CoO, as verified by XPS. The pore size is about 2 nm, and the CoO@Co nanoparticles were irregularly shaped and sized in the range of 20–300 nm, which may have been due to the aggregation of ultrafine nanoparticles. The existence of an interaction between the CoO@Co nanoparticles and the N-doped support is confirmed by XPS and H2-TPR. The catalyst shows superior activity for oxygen evolution reaction (OER) manifested in its lower charge potential (3.75 V at the current density of 100 mA g−1). Enhanced performances in coulombic efficiency, rate capability, and cycling stability (55 cycles) are also realized. Finally, these improvements, with the exception of the catalytic activity of CoO, may benefit from the interaction between the carbon supporter and the CoO@Co nanoparticles.
Co-reporter:Ruifeng Wang, Xiujuan Qi, Shimin Liu, Yude He, Youquan Deng
Journal of Molecular Liquids 2016 Volume 221() pp:339-345
Publication Date(Web):September 2016
DOI:10.1016/j.molliq.2016.05.092
•The possible impurities in the ionic liquids were measured.•Comparisons on the properties of the ionic liquids were systemically conducted.•The distinct changes in physicochemical properties were observed.•The reasons might be attributed to the impurities.A series of 1,3-dialkylimidazolium tetrafluoroborate salts had been prepared via one-step alkylation of N-alkylimidazole with trialkyloxonium salts and traditional two-step method, respectively. The possible impurities in these ionic liquids (ILs) such as Cl−, Br−, Na+ and alkyl imidazoles were measured. Detailed characterizations of two approaches in the ILs properties and performances such as spectroscopic properties, phase behavior, viscosity, refractive index, and electrochemical properties were systemically conducted. The obtained results showed that the variety of synthesized methods resulted in the distinct changes in physicochemical properties for the same IL. Therein, the comparison of spectroscopic properties and phase behaviors for the employed ILs were emphasized. Furthermore, in most cases, the ILs prepared by traditional two-step possessed the higher viscosity, lower refractive index as well as lower ionic conductivity than that of ILs prepared by one-step. It was worth noting that the 1-decyl-3-ethylimidazolium tetrafluoroborate ([DEIm]BF4) prepared with the traditional and trialkyloxonium methods respectively exhibited distinctly different phase and fluorescence behaviors. The reason might be attributed to the significant improvement on the purities of ILs by the one-step strategy.
Co-reporter:Peixue Wang, Xiangyuan Ma, Qinghe Li, Benqun Yang, Jianpeng Shang and Youquan Deng
RSC Advances 2016 vol. 6(Issue 59) pp:54013-54019
Publication Date(Web):31 May 2016
DOI:10.1039/C6RA07452A
A series of ionic liquids (P4,4,4,6BF4, P4,4,4,6Triz, as well as the newly prepared anion dual-functionalized amino-triz IL P4,4,4,6ATriz, etc.) were prepared, and their catalytic performance was tested in the synthesis of polyureas from CO2 and diamines. Under the optimized reaction conditions, good to excellent yields of various polyureas were achieved with different diamines over P4,4,4,6ATriz catalyst. It can be found that the catalytic performance is essentially consistent with the basicity of ILs (as determined by TPD method). The solid products were characterized extensively by 13C NMR, FT-IR, XRD, DSC and TGA. From these results, it could be concluded that the solid products based on diamines and CO2 have the polyurea structure with the urea linkage and connected by hydrogen bonds, which resulted in their high resistance to solvents and excellent thermal stability.
Co-reporter:Qinghe Li, Peixue Wang and Youquan Deng
RSC Advances 2016 vol. 6(Issue 47) pp:40890-40894
Publication Date(Web):12 Apr 2016
DOI:10.1039/C6RA05563J
A highly copper-catalysed amide exchange reaction of hexamethylenediamine (HDA) with CH3CN and H2O for the synthesis of hexamethylenebisacetamide (HMBA) without an organic solvent or gas protection was developed. 100% HDA conversion and >99% HMBA selectivity was obtained. X-ray diffraction, scanning emission microscopy, and temperature-programmed reduction of hydrogen were used to characterize the structural properties of the catalyst. The reaction mechanism was also investigated.
Co-reporter:Ruifeng Wang;Xiujuan Qi;Lei Zhao;Shimin Liu;Shuang Gao;Xiangyuan Ma
Journal of Separation Science 2016 Volume 39( Issue 13) pp:2444-2450
Publication Date(Web):
DOI:10.1002/jssc.201600170
Determination of methamphetamine in forensic laboratories is a major issue due to its health and social harm. In this work, a simple, sensitive, and environmentally friendly method based on ionic liquid dispersive liquid–liquid microextraction combined with high-performance liquid chromatography was established for the analysis of methamphetamine in human urine. 1-Octyl-3-methylimidazolium hexafluorophosphate with the help of disperser solvent methanol was selected as the microextraction solvent in this process. Various parameters affecting the extraction efficiency of methamphetamine were investigated systemically, including extraction solvent and its volume, disperser solvent and its volume, sample pH, extraction temperature, and centrifugal time. Under the optimized conditions, a good linearity was obtained in the concentration range of 10–1000 ng/mL with determination coefficient >0.99. The limit of detection calculated at a signal-to-noise ratio of 3 was 1.7 ng/mL and the relative standard deviations for six replicate experiments at three different concentration levels of 100, 500, and 1000 ng/mL were 6.4, 4.5, and 4.7%, respectively. Meanwhile, up to 220-fold enrichment factor of methamphetamine and acceptable extraction recovery (>80.0%) could be achieved. Furthermore, this method has been successfully employed for the sensitive detection of a urine sample from a suspected drug abuser.
Co-reporter:Peixue Wang, Yubo Ma, Shimin Liu, Feng Zhou, Benqun Yang and Youquan Deng
Green Chemistry 2015 vol. 17(Issue 7) pp:3964-3971
Publication Date(Web):02 Jun 2015
DOI:10.1039/C5GC01007A
The use of urea as an active form of carbon dioxide is a feasible way to substitute phosgene in the chemical industry. This paper reports an effective route for the synthesis of N-substituted carbamates from amines, urea and alcohols. Under the optimized reaction conditions, several important N-substituted carbamates were successfully synthesized in 95–98% yields over a TiO2–Cr2O3/SiO2 catalyst. The catalyst could be reused for several runs without deactivation. The catalysts were characterized by BET, XPS, XRD, and TPD, which suggested that the strength and amount of the acidic and basic sites might be the major reason for the high catalytic activity of TiO2–Cr2O3/SiO2.
Co-reporter:Benqun Yang, Qinghua Zhang, Yuqing Fei, Feng Zhou, Peixue Wang and Youquan Deng
Green Chemistry 2015 vol. 17(Issue 7) pp:3798-3805
Publication Date(Web):08 May 2015
DOI:10.1039/C5GC00691K
Utilization of cheap and natural resources is an important topic in green chemistry. A new class of betaine-based aprotic task-specific ionic liquids (ILs), including [C4bet][TFSI], [C4bet][DCA], [C4bet][SCN], [1O2bet][TFSI], [1O2bet][DCA], [2O2bet][TFSI], and [2O2bet][DCA], has been designed and prepared through a new ionic liquidization strategy from the renewable natural resource betaine. Their physicochemical characteristics, including spectral properties, density, viscosity, melting point, glass transition temperature, thermal stability, conductivity and electrochemical window, have been comprehensively studied. They were first applied as new absorbents for SO2 capture, and [C4bet][SCN] exhibited the maximum absorption capacity of 0.93 molSO2/molILs at 20 °C and 1 atm (SO2/N2 = 10% vol.) with rapid absorption rates in 21 min. Moreover, the effect of temperature, pressure, and water content on the absorption performance of SO2 was investigated. The possible absorption mechanism was studied using FT-IR, NMR and quantum chemical calculation. In addition, the [C4bet][SCN] can maintain the high absorption capacity and the rapid absorption rates for 25 absorption/desorption cycles.
Co-reporter:Xiaodong He, Qunfeng Shao, Pengfei Cao, Weijie Kong, Jiqian Sun, Xiaoping Zhang and Youquan Deng
Lab on a Chip 2015 vol. 15(Issue 5) pp:1311-1319
Publication Date(Web):02 Jan 2015
DOI:10.1039/C4LC01434K
An optofluidic waveguide with a simple two-terminal electrode geometry, when filled with an ionic liquid (IL), forms a lateral electric double-layer capacitor under a direct current (DC) electric field, which allows the realization of an extremely high carrier density in the vicinity of the electrode surface and terminals to modulate optical transmission at room temperature under low voltage operation (0 to 4 V). The unique electro-optical phenomenon of ILs was investigated at three wavelengths (663, 1330 and 1530 nm) using two waveguide geometries. Strong electro-optical modulations with different efficiencies were observed at the two near-infrared (NIR) wavelengths, while no detectable modulation was observed at 663 nm. The first waveguide geometry was used to investigate the position-dependent modulation along the waveguide; the strongest modulation was observed in the vicinity of the electrode terminal. The modulation phase is associated with the applied voltage polarity, which increases in the vicinity of the negative electrode and decreases at the positive electrode. The second waveguide geometry was used to improve the modulation efficiency. Meanwhile, the electro-optical modulations of seven ILs were compared at an applied voltage ranging from ±2 V to ±3.5 V. The results reveal that the modulation amplitude and response speed increase with increasing applied voltage, as well as the electrical conductivity of ILs. Despite the fact that the response speed isn't fast due to the high ionic density of ILs, the modulation amplitude can reach up to 6.0 dB when a higher voltage (U = ±3.5 V) is applied for the IL [Emim][BF4]. Finally, the physical explanation of the phenomenon was discussed. The effect of the change in IL structure on the electro-optical phenomena was investigated in another new experiment. The results reveal that the electro-optical phenomenon is probably caused mainly by the change in carrier concentration (ion redistribution near charged electrodes), which induces the enhancement and suppression of NIR optical absorption (contributed by C–H and N–H groups) in the vicinity of the negative electrode and positive electrode, respectively.
Co-reporter:Feng Zhou, Shimin Liu, Benqun Yang, Peixue Wang, Ahmad S. Alshammari, Youquan Deng
Electrochemistry Communications 2015 Volume 55() pp:43-46
Publication Date(Web):June 2015
DOI:10.1016/j.elecom.2015.03.015
•Excellent synergy was observed for the electrochemical reduction of CO2 to CO.•The electro-catalytic system exhibited continuous activity for more than 150 h.•The Faraday efficiency for CO formation was > 98%.In this study, the electrochemical reduction of CO2 was examined using a Ag-modified Cu catalyst cathode in a series of mixed ionic liquids (ILs) in the presence or absence of cobalt chloride (CoCl2). These results indicate that the Ag-modified Cu electrode in EMIMBF4 + BMIMNO3 with CoCl2 exhibited the excellent synergy for the electrochemical reduction of CO2 to CO with a stable area specific activity, with continuous production for at least 150 h. In such a system, a CO selectivity of 98% was achieved. According to the obtained results, a possible mechanism was proposed. The synergistic effect between the Ag-modified Cu electrode, serving as the main catalyst, and CoCl2 and ILs, serving as the co-catalysts, is probably responsible for the highly selective and stable electrocatalytic reduction of CO2 to CO.The electrochemical reduction of CO2 to CO over a silver-modified copper electrode in a mixed IL system of 24 g EMIMBF4 + 1 g BMIMNO3 (containing 0.25 mg CoCl2) exhibited excellent synergy with > 98% selectivity, and a stable area specific activity with continuous activity for at least 150 h.
Co-reporter:Benqun Yang, Feng Zhou, Shimin Liu, Peixue Wang, Ahmad S. Alshammari and Youquan Deng
RSC Advances 2015 vol. 5(Issue 60) pp:48908-48915
Publication Date(Web):27 May 2015
DOI:10.1039/C5RA08624H
A series of ionic liquids (P4,4,4,6BF4, APMIMBF4, P4,4,4,6Triz, as well as the newly prepared anion dual-functionalized amino-triz IL P4,4,4,6ATriz, etc.) supported on glass powder and SAPO-11 were prepared, and their interaction with CO2 was investigated by “limited” temperature-programmed desorption. The results showed that the strength of the interaction of CO2 with IL/glass powder (11 wt%) followed the order P4,4,4,6BF4 < APMIMBF4 < P4,4,4,6Triz < P4,4,4,6ATriz. Two desorption peaks were observed for P4,4,4,6Triz, probably attributed to the two sites of interaction between Triz and CO2, and the Gaussian 03 program was employed to obtain the optimized structures, revealing the interaction between P4,4,4,6Triz and CO2. When ILs were confined in the nanopores of SAPO-11, the desorption capacity and interaction strength increased because of the nano-confinement effect. Meanwhile, the loading, as well as the structure of ILs and Na2CO3-modified SAPO-11, significantly affected the interaction between CO2 and ILs. Besides, P4,4,4,6ATriz/SAPO-11 (modified with Na2CO3, 30 wt%) with a maximum CO2 desorption capacity of 1.55 moleCO2/moleILs could reversibly adsorb CO2 15 times without any apparent reduction in the desorption capacity.
Co-reporter:Peixue Wang, Shimin Liu, Xiangyuan Ma, Yude He, Ahmad S. Alshammari and Youquan Deng
RSC Advances 2015 vol. 5(Issue 33) pp:25849-25856
Publication Date(Web):06 Mar 2015
DOI:10.1039/C5RA02894A
Magnetic binary Mg–Fe oxides were prepared by a co-precipitation method, characterized and tested in the synthesis of ethyl methyl carbonate (EMC) from di methyl carbonate (DMC) and diethyl carbonate (DEC). The obtained results showed that the Mg/Fe oxide catalyst with a 1:1 molar ratio and calcined at 400 °C exhibited superior catalytic activity. The yield of EMC could reach 66% (at 100 °C for 1.5 h) with a TOF of 220 mmol h−1 gcat−1. The prepared catalysts could be magnetically separated, and reused for ten runs without noticeable deactivation. XRD and Mössbauer spectra revealed that there was a synergistic effect between Mg and Fe oxides in the catalysts, which was consistent with the results of TPR, i.e. the introduction of the Mg component favored the reduction of the Fe2O3. XPS and IR characterizations indicated that there were a large number of accessible Fe-OHs on the surface of MgFe-400, and combining the Fe-OHs with the basic MgO may be related to the highly catalytic performance.
Co-reporter:Peixue Wang, Shimin Liu, Feng Zhou, Benqun Yang, Ahmad S. Alshammari and Youquan Deng
RSC Advances 2015 vol. 5(Issue 103) pp:84621-84626
Publication Date(Web):01 Oct 2015
DOI:10.1039/C5RA17655G
Square-shaped Zn/Ti oxides were prepared by a co-precipitation method and used for the synthesis of diphenyl carbonate (DPC) via transesterification of dibutyl carbonate (DBC) with phenol. The results showed that a 51% yield of butyl phenyl carbonate (BPC) and 13% yield of DPC could be achieved at 205 °C in the presence of 3ZnTi-400 (Zn:Ti molar ratio 3:1). Moreover, it is found that 3ZnTi-400 was also an active catalyst for the disproportionation of BPC to DPC, and 80% conversion of BPC was obtained at 190 °C. The prepared catalysts could be reused for three runs of the transesterification without noticeable deactivation. The catalysts were characterized by XRD, SEM, XPS, and TPD with the aim of establishing the relationship between catalytic performance and structure.
Co-reporter:Peixue Wang, Shimin Liu, Liujin Lu, Xiangyuan Ma, Yude He and Youquan Deng
RSC Advances 2015 vol. 5(Issue 76) pp:62110-62115
Publication Date(Web):14 Jul 2015
DOI:10.1039/C5RA09281G
An efficient method using commercially available ionic liquids (ILs) as extractants for the separation of a close-boiling mixture containing dibutyl carbonate (DBC) and butyl carbamate (BC) was provided. It was found that 1-butyl-3-methylimidazolium chloride ([BMIM]Cl) displayed the best performance for the separation of DBC and BC, and the purity of the DBC and BC could reach 99.8% and 99.9%, respectively, under the optimum conditions. According to the results of infrared spectroscopy (IR) and thermogravimetric (TG) analyses, the superiority of [BMIM]Cl might be related to the high nucleophilicity (i.e. ability to hydrogen bond) of the Cl−, which could be able to interact with the amino in BC to form a eutectic mixture and resulted in easy removal of DBC. Meanwhile, no decomposition of [BMIM]Cl was observed in the heating process, and the obtained results showed that [BMIM]Cl could be successfully reused for ten recycles with DBC purity of 99.5% avoiding any further treatment. Moreover, [BMIM]Cl also exhibited good performance in the separation of a dimethyl carbonate/methanol azeotropic mixture.
Co-reporter:Peixue Wang, Shimin Liu, Feng Zhou, Benqun Yang, Ahmad S. Alshammari and Youquan Deng
RSC Advances 2015 vol. 5(Issue 25) pp:19534-19540
Publication Date(Web):11 Feb 2015
DOI:10.1039/C4RA15897K
The synthesis of diethyl carbonate (DEC) from urea and ethanol was carried out over Mg–Zn–Al composite oxide catalysts derived from hydrotalcites (HTs). The catalytic results showed that the ternary hydrotalcites calcined at 450 °C with Mg:Zn:Al = 1:1.7:1 exhibited superior catalytic activity, and the highest DEC yield was 67.8%. Similar to ethanol, other alcohols such as methanol and butanol can also be transformed to corresponding dialkyl carbonates. Catalysts were characterized by XRD, BET, SEM and TPD with the aim of establishing a relationship between performance and structure. The results indicated that MgZn1.7Al-450 with nanoplate morphology and more accessible active medium basic sites were favourable for obtaining much superior catalytic activity. Recycling experiments demonstrated that the catalyst could be successfully reused.
Co-reporter:Feng Zhou, Shimin Liu, Benqun Yang, Peixue Wang, Ahmad S. Alshammari, Youquan Deng
Electrochemistry Communications 2014 Volume 46() pp:103-106
Publication Date(Web):September 2014
DOI:10.1016/j.elecom.2014.06.023
•Metal Ag in BMImCl aqueous solution shows the excellent synergy.•The electro-catalytic system is relatively simple.•The electro-catalytic system presents better stability.•The selectivity of reduction of CO2 to CO (FE >99%) is higher.In this study, the electrochemical reduction of carbon dioxide (CO2) was examined in a series of aqueous solutions of ionic liquids on metal (silver (Ag), copper, platinum and gold) catalyst cathode. The results indicated that Ag metal cathode in 1-butyl-3-methylimidazolium chloride (BMImCl) with 20 wt.% water showed excellent synergy in electrochemical reduction of CO2 to carbon monoxide (CO) with extremely high selectivity (> 99%) and efficiency, and with stable area specific activity (ca. 2.4 mA·cm− 2). The behavior of electrocatalytic reduction of CO2 to CO on Ag electrode in ionic liquids (ILs) was examined by cyclic voltammogram. The study revealed that the chloride containing IL could be the most effective candidate for reduction of CO2 to CO and for inhibiting the hydrogen evolution reaction probably due to the dominated water–anion and water–cation interactions in aqueous BMImCl.The electrochemical reduction of CO2 to CO over metal Ag cathode in BMImCl aqueous solution showed the excellent synergy with > 99% selectivity and with stable area specific activity (ca. 2.4 mA·cm− 2).
Co-reporter:Peixue Wang, Shimin Liu, Feng Zhou, Benqun Yang, Ahmad S. Alshammari, Liujin Lu, Youquan Deng
Fuel Processing Technology 2014 Volume 126() pp:359-365
Publication Date(Web):October 2014
DOI:10.1016/j.fuproc.2014.05.012
•Zn/Y oxides with different precursors were prepared by co-precipitation method.•The synthesis of DMC via a two-step process uses urea, EG and methanol.•The catalyst with zinc nitrate precursor is highly active for the two processes.•The acid-base bifunctional Zn/Y oxides greatly enhance catalytic activity.•The interaction between Zn and Y oxides greatly enhance catalytic activity.The binary zinc-yttrium oxides with different precursors were prepared by co-precipitation method and used in the catalytic synthesis of dimethyl carbonate (DMC) via a two-step process using urea, ethylene glycol and methanol as raw feed-stocks. The first step involves reaction of urea with ethylene glycol (EG) to form ethylene carbonate (EC), and 96% conversion of urea with 98% selectivity of EC was obtained. In the second step, namely transesterification of EC formed with methanol to give DMC and EG, the conversion of EC was up to 72% in 15 min with a 99% selectivity of DMC, corresponding to a TOF of 864 mmol/h gcat. XRD results showed that the catalyst with a zinc nitrate precursor has a remarkable interaction between zinc and yttrium oxides. TPD characterization indicated that in the catalyst with a zinc nitrate precursor there was a cooperative effect between weak acid and medium base sites on the surface of the catalyst, suggesting that the prepared catalysts are acid–base bifunctional. The synergistic effect between zinc and yttrium oxides, in combination with acidity of zinc oxide and basicity of yttrium oxide, may be responsible to the high catalytic activity and selectivity.
Co-reporter:Weijie Kong, Pengfei Cao, Xiaodong He, Long Yu, Xiangyuan Ma, Yude He, Liujin Lu, Xiaoping Zhang and Youquan Deng
RSC Advances 2014 vol. 4(Issue 37) pp:19356-19361
Publication Date(Web):26 Feb 2014
DOI:10.1039/C4RA00629A
This paper presents an ionic liquid based vibrational energy harvester by periodically squeezing the liquid bridge, which has excellent characteristics such as the lack of a requirement for an airtight space, stability over a wide operating temperature range (up to 100 °C) and in particular improved output power at high temperatures.
Co-reporter:Xiaodong He, Qunfeng Shao, Weijie Kong, Long Yu, Xiaoping Zhang, Youquan Deng
Fluid Phase Equilibria 2014 Volume 366() pp:9-15
Publication Date(Web):25 March 2014
DOI:10.1016/j.fluid.2014.01.003
An optofluidic method based on a liquid-core and liquid-cladding optical waveguide is proposed for roughly estimating the extent of diffusive mixing between two fluids. The mutual diffusion coefficient was estimated from a charged coupled device (CCD) camera image of light-focusing in accordance with predictions of a three-dimensional model. To check the validity of our proposed method, mutual diffusion coefficients of aqueous solutions of ethylene glycol at different volume fractions were measured, firstly. Then, mutual diffusion coefficients of eight 1,3-methylimidazolium ionic liquids-water binary systems were estimated at 298.2 K. Our results show that the mutual diffusion coefficients, in order of decreasing values, are as follows: [Emim][N(CN)2] > [Mmim][BF4] > [Emim][BF4] > [Bmim][NO3] > [Bmim][N(CN)2] > [Emim][ClO4] > [Bmim][BF4] > [Bmim][ClO4], it is well correlated to molecular weights of the ionic liquids. Finally, mutual diffusion coefficients of three ionic liquids-water binary systems at temperatures ranging from 298.2 to 338.2 K were measured, which is sensitive to temperature and increases quickly with it. Our results show a moderate discrepancy, but this proposed optofluidic method allows one to perform diffusion measurements with a simple, costless and microlitre volume manner in highly confined spaces.We reported an optofluidic approach for estimating mutual diffusion coefficients of ionic liquids-water binary systems based on a liquid-core and liquid-cladding optical waveguide.
Co-reporter:Ying Wang, Xiaojian Lu, Yu Liu, Youquan Deng
Electrochemistry Communications 2013 Volume 31() pp:108-111
Publication Date(Web):June 2013
DOI:10.1016/j.elecom.2013.03.017
•Ag/Co3O4–C was firstly used for oxygen reduction in alkaline media.•The ORR activity of Ag/Co3O4–C was higher than those of Ag/C and Co3O4–C catalysts.•Ag/Co3O4–C showed better methanol tolerance and stability in alkaline media than Pt/C.The electroreduction of oxygen was firstly studied on Ag/Co3O4–C in alkaline media prepared by depositing Ag on Co3O4 modified carbon (Co3O4–C). The Ag/Co3O4–C composite not only displayed relatively large electrochemical active surface area (ESA), high catalytic activity towards oxygen reduction reaction (ORR), but also exhibited good methanol tolerance and stability in alkaline media. Ag/Co3O4–C could be a valuable catalyst for ORR and be applied to alkaline fuel cells and metal–air batteries.
Co-reporter:Shiguo Zhang, Yan Zhang and Youquan Deng
RSC Advances 2013 vol. 3(Issue 29) pp:11480-11484
Publication Date(Web):16 May 2013
DOI:10.1039/C3RA41190G
Electric fields of ionic liquids (ILs) were investigated by vibrational Stark effect spectroscopy using ethyl thiocyanate as a probe molecule. It was found that the stretching vibration of CN in nonhydroxyl ILs originates exclusively from the intrinsic electric fields, which are on average 3.0 MV cm−1 higher than those of molecular solvents. In contrast, in the case of hydroxyl functional ILs, hydrogen bonding as well as the electric field contribute to the IR shift of CN.
Co-reporter:Ying Wang, Xiangyuan Ma, Liujin Lu, Yude He, Xiujuan Qi, Youquan Deng
International Journal of Hydrogen Energy 2013 Volume 38(Issue 31) pp:13611-13616
Publication Date(Web):17 October 2013
DOI:10.1016/j.ijhydene.2013.08.048
•MnOx–Co3O4/C was firstly used for oxygen reduction in alkaline media.•The ORR activity of MnOx–Co3O4/C was higher than those of MnOx/C and Co3O4/C.•MnOx–Co3O4/C showed better methanol tolerance and stability than Pt/C.The electroreduction of oxygen of MnOx–Co3O4/C was firstly studied in alkaline media. The MnOx–Co3O4/C showed better electrocatalytic activity towards ORR than MnOx/C and Co3O4/C. Compared to Pt/C, MnOx–Co3O4/C showed better methanol tolerance and durability in alkaline solution. Thus, the MnOx–Co3O4/C catalyst had potential for applications in metal–air batteries and alkaline fuel cells.
Co-reporter:Shiguo Zhang, Yan Zhang, Xiangyuan Ma, Liujin Lu, Yude He, and Youquan Deng
The Journal of Physical Chemistry B 2013 Volume 117(Issue 9) pp:2764-2772
Publication Date(Web):February 11, 2013
DOI:10.1021/jp312251q
Because of its sensitivity to chemical and electrostatic characteristics, nitrile group as an infrared (IR) probe to monitor the local structure, folding kinetics, and electrostatic environment of protein, or solvation of molecular solvents, has attracted increasing attention. Herein, by choosing benzonitrile and imidazolium ionic liquids (ILs) as the IR probe and model ILs, respectively, we report that the nitrile stretching vibration (νCN) could be utilized as a simple and substantial IR probe to monitor the local environment of ILs such as hydrogen bonding (H-bonding) as well as intrinsic electric field. In 1-alkyl-3-methylimidazolium-based non-hydroxyl ILs, the νCN is in a “free” state, and is less affected by the alkyl chain, while it significantly decreases with the effective anion charge. In 1-(2-hydroxyethyl)-3-methylimidazolium-based hydroxyl ILs, however, a distinct anion-dependent νCN forming H-bonding with the hydroxyl is also observed besides the “free” νCN band. The “free” component of νCN can be further employed to determine the intrinsic electric field in both non-hydroxyl (directly) and hydroxyl (indirectly by subtracting H-bonding contribution) ILs by using vibrational Stark effect. Moreover, the result suggests that benzonitrile is preferentially located in the charge domain in ILs and it could be a more suitable probe to report the ionic network rather than the nonpolar domain in ILs.
Co-reporter:Jianpeng Shang, Shimin Liu, Xiangyuan Ma, Liujin Lu and Youquan Deng
Green Chemistry 2012 vol. 14(Issue 10) pp:2899-2906
Publication Date(Web):08 Aug 2012
DOI:10.1039/C2GC36043H
This paper reports an effective route for the syntheses of N-substituted dicarbamates from dialkyl carbonates and polyurea derivatives, in which polyurea derivatives could be successfully synthesized from aliphatic diamines and CO2 in the absence of any catalyst. Under the optimized reaction conditions, various N-substituted carbamates were successfully synthesized with 93–98% isolated yields over a MgO–ZnO catalyst. The catalyst could be reused for several runs without deactivation. The catalysts were characterized with X-ray photoelectron spectroscopy, X-ray diffraction and temperature-programmed desorption.
Co-reporter:Shiguo Zhang, Yan Zhang, Ying Wang, Shimin Liu and Youquan Deng
Physical Chemistry Chemical Physics 2012 vol. 14(Issue 15) pp:5132-5138
Publication Date(Web):13 Feb 2012
DOI:10.1039/C2CP23675C
Ionic liquids (ILs)-stabilized iron oxide (Fe2O3) nanoparticles were synthesized by the ultrasonic decomposition of iron carbonyl precursors in [EMIm][BF4] without any stabilizing or capping agents. The Fe2O3 nanoparticles were isolated and characterized by X-ray powder diffraction, transmission electron microscopy and susceptibility measurements. The physicochemical properties of ILs containing magnetic Fe2O3 nanoparticles (denoted as Fe2O3@[EMIm][BF4]), including surface properties, density, viscosity and stability, were investigated in detail and compared with that of [EMIm][BF4]. The Fe2O3@[EMIm][BF4] can be directly used as magnetic ionic liquid marble by coating with hydrophobic and unreactive polytetrafluoroethylene (PTFE), for which the effective surface tension was determined by the puddle height method. The resulting magnetic ionic liquid marble can be transported under external magnetic actuation, without detachment of magnetic particles from the marble surface that is usually observed in water marble.
Co-reporter:Shiguo Zhang, Zhengjian Chen, Xiujuan Qi and Youquan Deng
New Journal of Chemistry 2012 vol. 36(Issue 4) pp:1043-1050
Publication Date(Web):15 Feb 2012
DOI:10.1039/C2NJ20965A
The polarity of ionic liquids (ILs), usually denoted as ET(30) by the solvatochromic probe Reichardt’s dye, is one of the most fundamental properties that remarkably affect the solvation and chemical reaction in ILs. It was generally accepted that the ET(30) of ILs was dominated by the nature of the cation. However, in this work, it was found that the common ammonium-based ILs showed strongly anion-dependent ET(30). For example, the ET(30) value for [N1124][DCA] and [N1124][NTf2] is 49.0 and 59.0 kcal mol−1, respectively, while the corresponding imidazolium ILs bearing the same anions possess nearly identical ET(30), the ET(30) value for [BMIm][DCA] and [BMIm][NTf2] is 51.4 and 51.6 kcal mol−1, respectively. Moreover, introduction of an ether group was found to increase the ET(30) of imidazolium ILs while having no obvious effect on that of ammonium-based ILs. The Kamlet–Taft parameters and density functional theory (DFT) calculations indicated that the distinct result is related to different stabilization of the ground state of Reichardt's dye 30. In imidazolium ILs, the main interactions between ILs and zwitterionic dye involve both coulombic interaction (between the cation and the phenolate oxygen atom) and H-bonding interaction (between the acidic hydrogen on imidazolium ring and the phenolate oxygen atom). However, with the ammonium ILs lack of active hydrogen, the dye is only stabilized by the coulombic interaction between the cation and the phenolate oxygen atom. Interestingly, in both imidazolium and ammonium-based ILs, the spiropyran–merocyanine equilibrium exhibit obvious anion-dependent photochromism, solvatochromism, and thermal relaxation.
Co-reporter:Shiguo Zhang;Xiujuan Qi;Xiangyuan Ma;Liujin Lu;Qinghua Zhang
Journal of Physical Organic Chemistry 2012 Volume 25( Issue 3) pp:248-257
Publication Date(Web):
DOI:10.1002/poc.1901
Gas-phase structure, hydrogen bonding, and cation–anion interactions of a series of 1-(2-hydroxyethyl)-3-methylimidazolium ([HOEMIm]+)-based ionic liquids (hereafter called hydroxyl ILs) with different anions (X = [NTf2]–, [PF6]–, [ClO4]–, [BF4]–, [DCA]–, [NO3]–, [AC]– and [Cl]–), as well as 1-ethyl-3-methylimizolium ([EMIm]+)-based ionic liquids (hereafter called nonhydroxyl ILs), were investigated by density functional theory calculations and experiments. Electrostatic potential surfaces and optimized structures of isolated ions, and ion pairs of all ILs have been obtained through calculations at the Becke, three-parameter, Lee–Yang–Parr/6-31 + G(d,p) level and their hydrogen bonding behavior was further studied by the polarity and Kamlet–Taft Parameters, and 1H-NMR analysis. In [EMIm]+-based nonhydroxyl ILs, hydrogen bonding preferred to be formed between anions and C2–H on the imidazolium ring, while in [HOEMIm]+-based hydroxyl ILs, it was replaced by a much stronger one that preferably formed between anions and OH. The O–H···X hydrogen bonding is much more anion-dependent than the C2–H···X, and it is weakened when the anion is changed from [AC]– to [NTf2]–. The different interaction between [HOEMIm]+ and variable anion involving O–H···X hydrogen bonding resulted in significant effect on their bulk phase properties such as 1H-NMR shift, polarity and hydrogen-bond donor ability (acidity, α). Copyright © 2011 John Wiley & Sons, Ltd.
Co-reporter:Dr. Shiguo Zhang;Dr. Shimin Liu;Dr. Yan Zhang ; Youquan Deng
Chemistry – An Asian Journal 2012 Volume 7( Issue 9) pp:2004-2007
Publication Date(Web):
DOI:10.1002/asia.201200417
Co-reporter:Shiguo Zhang;Rui Shi;Xiangyuan Ma;Liujin Lu;Yude He;Xiaohu Zhang; Yanting Wang; Youquan Deng
Chemistry - A European Journal 2012 Volume 18( Issue 38) pp:
Publication Date(Web):
DOI:10.1002/chem.201290163
Co-reporter:Shiguo Zhang;Rui Shi;Xiangyuan Ma;Liujin Lu;Yude He;Xiaohu Zhang; Yanting Wang; Youquan Deng
Chemistry - A European Journal 2012 Volume 18( Issue 38) pp:11904-11908
Publication Date(Web):
DOI:10.1002/chem.201201257
Co-reporter:Qinghua Zhang, Shiguo Zhang and Youquan Deng
Green Chemistry 2011 vol. 13(Issue 10) pp:2619-2637
Publication Date(Web):23 Aug 2011
DOI:10.1039/C1GC15334J
Due to their unique properties, ionic liquids have offered great potential for developing clean catalytic technologies. After a short introduction of their advantages in green catalysis, recent advances in ionic liquid catalysis are reviewed with emphasis on four hot fields, viz. biomass conversion in ionic liquids, catalytic production of fine chemicals in ionic liquids, supported ionic liquid phase catalysis, as well as Friedel–Crafts reactions in ionic liquids. In particular, through selected samples, we show here the advantages and potential of ionic liquids in exploring cleaner catalytic technologies, as compared to traditional catalytic processes. Finally, further development of ILs in catalysis is briefly prospected.
Co-reporter:Qinghua Zhang, Xiangyuan Ma, Shimin Liu, Benqun Yang, Liujin Lu, Yude He and Youquan Deng
Journal of Materials Chemistry A 2011 vol. 21(Issue 19) pp:6864-6868
Publication Date(Web):05 Apr 2011
DOI:10.1039/C1JM10491H
Nine 1-allyl-3-alkylimidazolium ([ACnIm]) or 1-vinyl-3-alkylimidazolium ([VCnIm]) dicyanamides (DCA) were prepared and characterized, and their physicochemical properties were studied in detail. Except for [AVIm]DCA and [AC4Im]DCA, the other dicyanamides with hexyl or longer alkyl chains on the cation exhibited the characteristic of hydrophobicity. Among them, [AC8Im]DCA and [AC10Im]DCA were found to possess similar densities to water, i.e. 1.007 g cm−3 and 0.988 g cm−3 at 25 °C, respectively. Interestingly, a reversible phase reversion of a [AC8Im]DCA/H2O mixture was observed as the temperature varied. These environmentally-friendly liquid materials have potential applications as precursors for syntheses of conducting polymeric materials.
Co-reporter:Zhengjian Chen, Shiguo Zhang, Xiujuan Qi, Shimin Liu, Qinghua Zhang and Youquan Deng
Journal of Materials Chemistry A 2011 vol. 21(Issue 25) pp:8979-8982
Publication Date(Web):27 May 2011
DOI:10.1039/C1JM11556A
Quinolizinium ionic liquids (salts) featuring an unbranched cation core have been prepared, characterized and found to show extremely high fluorescence quantum yields in solution (Φf > 99%, λem near 334 nm) and bright cyan fluorescence in molten state (λem near 465 nm).
Co-reporter:Qinghua Zhang, Benqun Yang, Shiguo Zhang, Shimin Liu and Youquan Deng
Journal of Materials Chemistry A 2011 vol. 21(Issue 41) pp:16335-16338
Publication Date(Web):20 Sep 2011
DOI:10.1039/C1JM13828F
A new class of liquid fluorescent organic salts was designed and prepared through via a strategy of ionic liquidization. These new ionic liquid materials exhibited strong green fluorescence and remarkable solvent-dependent photoluminescence under UV irradiation. Their physicochemical properties, especially the fluorescent behaviour, were studied intensively.
Co-reporter:Shiguo Zhang, Shimin Liu, Qinghua Zhang and Youquan Deng
Chemical Communications 2011 vol. 47(Issue 23) pp:6641-6643
Publication Date(Web):12 May 2011
DOI:10.1039/C1CC11924A
A new class of azobenzene-based photoresponsive ionic liquids was prepared and showed reversible modulation of ionic conductivity in specific solvents under alternative UV/visible light irradiation.
Co-reporter:Qinghua Zhang, Shiguo Zhang, Shimin Liu, Xiangyuan Ma, Liujin Lu and Youquan Deng
Analyst 2011 vol. 136(Issue 7) pp:1302-1304
Publication Date(Web):08 Feb 2011
DOI:10.1039/C0AN00885K
Six ionic liquid (IL)-modified dyes were synthesized and characterized. Compared to the methyl red and methyl orange, these IL-modified [MR]−- or [MO]−-based dyes exhibit lower melting points and enhanced solubility, and can be used as sensitive indicators towards free proton in both aqueous and non-aqueous solutions. This work also supplies a new concept of developing novel modified materials with the ILs.
Co-reporter:Xiaodong Hu, Shiguo Zhang, Chao Qu, Qinghua Zhang, Liujin Lu, Xiangyuan Ma, Xiaoping Zhang and Youquan Deng
Soft Matter 2011 vol. 7(Issue 13) pp:5941-5943
Publication Date(Web):02 Jun 2011
DOI:10.1039/C1SM05585B
This work presents ionic liquid based variable focus lenses using electrowetting, which exhibit excellent performance over a conventional saline based lens such as good tolerance of sharp temperature variation, wide operating temperature range (which is up to 100 °C) and in particular high stability at high temperatures.
Co-reporter:Shimin Liu;Zhengjian Chen;Qinghua Zhang;Shiguo Zhang;Zuopeng Li;Feng Shi;Xiangyuan Ma
European Journal of Inorganic Chemistry 2011 Volume 2011( Issue 12) pp:1910-1920
Publication Date(Web):
DOI:10.1002/ejic.201001351
Abstract
A new series of low-melting ammonium salts based on the [nido-7,8-C2B9H12]– anion have been synthesized and characterized, and their physicochemical properties including spectroscopic properties, thermal properties, surface properties, solubility, density, viscosity, electrochemical properties, and tribological properties have been studied in detail. In comparison with previously reported carborane-derivatized imidazolium or pyridinium salts, these diether-functionalized ammonium salts display lower phase transition temperatures (Tg = –76 to –57 °C), and four exist as liquids at room temperature due to their flexible alkoxy chains. TGA analysis revealed that the weight loss rates of these carborane-derivatized low-melting salts were ca. 30–80 wt.-% after thermal decomposition, which is different from the traditional RTILs. SEM images showed that the resulting residue had hollow reticular shell morphology, and XPS and XRD analyses indicate that the main components of the skeleton are B2O3 and amorphous carbon. This provides a new strategy for preparing new inorganic porous materials by thermal decomposition of these low-melting salts.
Co-reporter:Zhengjian Chen, Shimin Liu, Zuopeng Li, Qinghua Zhang and Youquan Deng
New Journal of Chemistry 2011 vol. 35(Issue 8) pp:1596-1606
Publication Date(Web):25 May 2011
DOI:10.1039/C1NJ20062C
A series of new ionic liquids, based on dialkoxy-functionalized quaternary ammonium cations {side chains: 1 = CH3, 1O1 = CH3OCH2, 1O2 = CH3OC2H4, 2O2 = C2H5OC2H4; cations: [N11,1O1,1O2], [N11,1O1,2O2], [N11,1O2,1O2], [N11,1O2,2O2] and [N11,2O2,2O2]}, with BF4−, (CF3SO2)2N− (NTf2) and CH3CO2− (OAc) as counteranions, have been prepared and characterized. Their basic properties, such as spectroscopic characteristics, melting point, glass transition temperature, thermal stability, electrochemical window, density, refractive index, viscosity and conductivity, were measured and comparatively studied. The incorporation of two flexible alkoxy chains makes the quaternary ammonium salts highly qualified to be low-viscous and high-conductive room temperature ILs, and even some of them have significantly better fluidity than the popular imidazolium ILs with a similar molecular weight, e.g.[N11,1O1,2O2]BF4 (151 cP and 2.11 mS cm−1, Mw: 249) vs.[HMIm]BF4 (220 cP and 1.2 mS cm−1, Mw: 256) at 25 °C. The electrochemical windows of these ILs were evaluated up to 5.5 V. In addition, the dialkoxy OAc ILs were found to have excellent solvent power for cellulose under mild conditions, e.g. a solution of 18 wt% microcrystalline cellulose in [N11,2O2,2O2]OAc at 80 °C. By precipitation with water, the dissolved cellulose (I crystal structure) was regenerated as nanosized cellulose II particles with increased surface area and decreased crystallinity, determined by FE-SEM and XRD.
Co-reporter:Jian Li;Liguo Wang;Feng Shi;Shimin Liu;Yude He;Liujin Lu
Catalysis Letters 2011 Volume 141( Issue 2) pp:339-346
Publication Date(Web):2011 February
DOI:10.1007/s10562-010-0498-6
One kind of novel ionic liquids (ILs) with a tertiary amino moiety and a quaternary ammonium group were synthesized and identified by FT-IR, 1H and 13C NMR. The elemental chemical state and basicity of ILs were determined by XPS and Hammett indicator method, respectively. Then the catalytic performance of these bi-functional catalysts was investigated in one-step synthesis of dimethyl carbonate (DMC) from ethylene oxide (EO), carbon dioxide and methanol. The best catalytic performance with 99% EO conversion and a maximum of 74% DMC selectivity was obtained using [N111,6N11]I as catalyst under optimized reaction conditions. And the catalyst could be reused for several times. Normally, stronger basicity could be obtained by altering the anions with different nucleophilicity in ILs and a better catalytic activity could be achieved correspondingly. A mechanism that both the ring opening of epoxide through nucleophilic attacks and the transesterification play an important role in the reaction was proposed based on experimental results.
Co-reporter:Xiaoguang Guo;Jianpeng Shang;Jian Li;Liguo Wang;Yubo Ma;Feng Shi
Chinese Journal of Chemistry 2010 Volume 28( Issue 2) pp:164-170
Publication Date(Web):
DOI:10.1002/cjoc.201090048
Abstract
A series of silica gel immobilized lanthanum catalysts were prepared for the atom-economy synthesis of N-substituted carbamates from urea derivatives and dimethyl carbonate. The La/SiO2 catalysts with lanthanum loadings varied from 1.3 wt% to 8.5 wt% were characterized by AES, BET, XRD, TEM, FT-IR, XPS and TPD. According to the characterization, lanthanum species with particle sizes of 5–10 nm on the surface of silica gel were formed. The catalysts were all amorphous and the surface areas were 336.5–530.2 m2/g. NH3-TPD analysis showed that all samples exhibited similar acid strength with different acid amounts. FT-IR measurement indicated that the component of lanthanum species on the catalyst surface were La(OH)3, LaOOH and hydrated La2O3. Also, the peak value of the absolute amount of LaOOH was obtained with 4.3 wt% lanthanum loading. The BET surface area decreased dramatically when the lanthanum loading was above 4.3 wt%. In consideration of the results obtained from the catalytic reactions, it could be concluded that LaOOH was the possible active species and high surface area was important for the high catalytic activity.
Co-reporter:Xinjiang Cui, Feng Shi, Yan Zhang, Youquan Deng
Tetrahedron Letters 2010 Volume 51(Issue 15) pp:2048-2051
Publication Date(Web):14 April 2010
DOI:10.1016/j.tetlet.2010.02.056
Co-reporter:Xinjiang Cui;Shiguo Zhang;Dr. Feng Shi;Dr. Qinghua Zhang;Xiangyuan Ma;Liujin Lu; Youquan Deng
ChemSusChem 2010 Volume 3( Issue 9) pp:1043-1047
Publication Date(Web):
DOI:10.1002/cssc.201000075
Co-reporter:Shiguo Zhang, Xiujuan Qi, Xiangyuan Ma, Liujin Lu and Youquan Deng
The Journal of Physical Chemistry B 2010 Volume 114(Issue 11) pp:3912-3920
Publication Date(Web):March 3, 2010
DOI:10.1021/jp911430t
The polarity of a series of ionic liquids (ILs) based on hydroxyethyl-imidazolium moiety with various anions ([PF6], [NTf2], [ClO4], [DCA], [NO3], [AC], and [Cl]) and their corresponding nonhydroxyl ILs was investigated by solvatochromic dyes and fluorescence probe molecules. Most of the nonhydroxyl ILs exhibit anion-independent polarity with similar ET(30) in the narrow range of 50.7−52.6 kcal/mol, except [EMIm][AC] (49.7 kcal/mol). However, the polarity of the hydroxyl ILs covers a rather wide range (ET(30) = 51.2−61.7 kcal/mol) and is strongly anion-dependent. According to their ET(30) or ET(33) values, the hydroxyl ILs can be further classified into the following three groups: (Ι) acetate-based hydroxyl ILs [HOEMIm][AC] exhibit polarity scale (ET(30) = 51.2 kcal/mol) similar to short chain alcohol and fall in the range of the nonhydroxyl ILs; (II) Hydroxyl ILs containing anions [NO3], [DCA], and [Cl] exhibit comparable polarity (ET(30) = 55.5−56.9 kcal/mol), moderately higher than those of their nonhydroxyl ILs; (III) Hydroxyl ILs containing anions [PF6], [NTf2], and [ClO4] possess unusual “hyperpolarity” (ET(30) = 60.3−61.7 kcal/mol) close to protic ILs and water. Kamlet−Taft parameters and density functional theory calculations indicated that the greatly expanded range of polarity of hydroxyl ILs is correlated to an intramolecular synergistic solvent effect of the ionic hydrogen-bonded HBD/HBA complexes generated by intrasolvent HBD/HBA association between the anions and the hydroxyl group on cations, wherein hydroxyl group exhibits a significant differentiating effect on the strength of H-bonding and thus the polarity. Spiropyran-merocyanine equilibrium acted as a model polarity-sensitive reaction indeed shows obviously polarity-dependent solvatochromism, photochromism, and thermal reversion in hydroxyl ILs.
Co-reporter:Jian Li;XiaoGuang Guo;LiGuo Wang;XiangYuan Ma;QingHua Zhang
Science China Chemistry 2010 Volume 53( Issue 7) pp:1534-1540
Publication Date(Web):2010 July
DOI:10.1007/s11426-010-4026-8
A base-free catalyst system Co(acac)3/BMMImCl was developed for the carbonylation of amines with CO2. 45%\2-81% isolated yields for N,N-dialkylureas and 6%\2-23% isolated yields for N,N-diarylureas were obtained. The catalyst system was recovered and reused without significant loss in activity. In this catalyst system, the base catalyst and chemical dehydrant were efficiently avoided. Different reaction conditions were also discussed and a postulated mechanism was proposed.
Co-reporter:Shiguo Zhang Dr.;Xiaodong Hu Dr.;Chao Qu;Qinghua Zhang;Xiangyuan Ma;Liujin Lu;Xueli Li;Xiaoping Zhang
ChemPhysChem 2010 Volume 11( Issue 11) pp:2327-2331
Publication Date(Web):
DOI:10.1002/cphc.201000290
Co-reporter:Xueli Li;Xiangyuan Ma;Feng Shi
ChemSusChem 2010 Volume 3( Issue 1) pp:71-74
Publication Date(Web):
DOI:10.1002/cssc.200900218
Co-reporter:Lequan Liu, Botao Qiao, Yude He, Feng Zhou, Benqun Yang, Youquan Deng
Journal of Catalysis (October 2012) Volume 294() pp:29-36
Publication Date(Web):1 October 2012
DOI:10.1016/j.jcat.2012.06.018
Co-oxidation of CO and H2 or oxidation of H2 in the presence of CO was first achieved at low temperatures (0–20 °C) over single-component catalysts (Pd/FeOx) at a space velocity of 15,000mlgcat-1h-1. A systematical study of FeOx- and Al2O3-supported Pd catalysts is carried out by means of STEM, TEM, XRD, XPS, Mössbauer spectra, and time-resolved CO titration. Highly dispersed Pd nanoparticles with size 1–1.8 nm over 5.4 wt% Pd/FeOx are confirmed by HAADF-STEM and HRTEM. Time-resolved CO titration, Mössbauer spectra, and XRD and XPS results suggest FeOx support supplying active oxygen is involved in the oxidations. Particle size effect and oxygen supply from FeOx support are speculated to be the main reasons for the excellent performance of Pd/FeOx in co-oxidation of CO and H2 or oxidation of H2 in the presence of CO.Graphical abstractCo-oxidation of CO and H2 or oxidation of H2 in the presence of CO was achieved at low temperatures (0–20 °C) over single-component catalysts (Pd/FeOx) at a space velocity of 15,000mlgcat-1h-1. Based on a systematical characterization study, it is speculated that highly dispersed Pd nano particles and FeOx support supplying active oxygen which is involved in oxidations are the key factors for excellent performance of Pd/FeOx for co-oxidation of CO and H2 at low temperatures.Download high-res image (160KB)Download full-size imageHighlights► Co-oxidation of CO and H2 or oxidation of H2 in the presence of CO was achieved at low temperatures (0–20 °C). ► Particle size effect is evident. ► Highly dispersed Pd nano particles over Pd/FeOx are indispensable but not enough for high co-oxidation activity. ► FeOx support supplying active oxygen is involved in oxidations. ► Time-resolved CO titration.
Co-reporter:Xue-li LI, Feng SHI, Xiang-yuan MA, Liu-jin LU, You-quan DENG
Journal of Fuel Chemistry and Technology (October 2010) Volume 38(Issue 5) pp:544-553
Publication Date(Web):1 October 2010
DOI:10.1016/S1872-5813(10)60043-6
AbstractEffect of ionic liquids (ILs) as media for the decomposition of formic acid in the presence of organic amine was investigated, and this activity was observed to be markedly promoted by the addition of ILs, especially for BMImCl. Based on this finding and to avoid volatile organic amine, a series of amine-functionalized ILs were further designed and prepared as both reaction media and co-catalyst for homogeneous decomposition of formic acid. Among the ILs investigated, i-Pr2NEMImCl-HCOONa system exhibited high activity (TOF > 600 mol/mol/h). This efficient and green method to produce hydrogen by formic acid decomposition has practical potentiality.
Co-reporter:Liguo Wang, Ying Wang, Shimin Liu, Liujin Lu, Xiangyuan Ma, Youquan Deng
Catalysis Communications (30 November 2011) Volume 16(Issue 1) pp:45-49
Publication Date(Web):30 November 2011
DOI:10.1016/j.catcom.2011.09.004
The binary zinc–yttrium oxides were prepared by co-precipitation method, characterized and tested in the synthesis of DMC via transesterification of ethylene carbonate with methanol. The catalytic results showed that the catalyst with Zn/Y molar ratio of 3 and calcined at 400 °C exhibited superior catalytic activity, corresponding to TOF of 236 mmol/gcat h. Appropriate content of yttrium in the catalyst enhanced the catalytic activity remarkably. Moreover, the abundance of medium basic sites (7.2 < H_ < 9.8, as determined by Hammett indicator method) was considered to be responsible for the superior catalytic activity.Binary zinc–yttrium oxides were prepared by co-precipitation method and found to catalyze the DMC synthesis from ethylene carbonate and methanol with high efficiency.Download full-size imageHighlights► Binary zinc-yttrium oxides were prepared by co-precipitation. ► Zn3Y-400 exhibited higher catalytic activity in DMC synthesis from EC and methanol. ► Optimal content of yttrium in the catalyst enhanced the catalytic activity greatly. ► The catalytic activity essentially correlated with the medium basicity.
Co-reporter:Jianpeng Shang, Xiaoguang Guo, Feng Shi, Yubo Ma, Feng Zhou, Youquan Deng
Journal of Catalysis (25 April 2011) Volume 279(Issue 2) pp:328-336
Publication Date(Web):25 April 2011
DOI:10.1016/j.jcat.2011.01.030
A series of catalysts of magnetic iron oxide containing Ni with different nickel content were prepared with co-precipitation method and tested in the syntheses of N-substituted carbamates from various amines and alkyl carbamates. Under the optimized reaction conditions, various N-substituted carbamates were successfully synthesized with 90–98% isolated yield. The catalyst could be recovered based on the magnetic property of the catalyst and reused for five runs without deactivation. The catalysts were characterized with X-ray photoelectron spectroscopy, X-ray diffraction, temperature-programmed reduction, temperature-programmed desorption, and Mössbauer spectroscopy analyses. The results showed that the catalytic activity may be derived from the delicate synergy between Ni and Fe species resulted in specific basic sites. Quasi in situ FT-IR and isotopic tracer revealed that the formation of substituted urea was the key step and the N-substituted carbamate was formed via further alcoholysis of the substituted urea.Graphical abstractA magnetic Ni/Fe3O4 catalyst was developed for the syntheses of N-substituted carbamates with amines and alkyl carbamates. Reaction pathway investigation revealed that the N-substituted carbamate was formed via urea intermediate.Download high-res image (81KB)Download full-size imageResearch highlights► Ni/Fe3O4 catalyst was developed for the N-substituted carbamates synthesis. ► N-substituted carbamate was formed via urea intermediate. ► Catalytic activity was derived from the delicate synergy between Ni and Fe species.
Co-reporter:Lequan Liu, Feng Zhou, Liguo Wang, Xiujuan Qi, Feng Shi, Youquan Deng
Journal of Catalysis (19 August 2010) Volume 274(Issue 1) pp:1-10
Publication Date(Web):19 August 2010
DOI:10.1016/j.jcat.2010.05.022
A series of FeOx- and Al2O3-supported Pt, Pd catalysts (0.23–2.1%) were prepared in this study. Pt/FeOx exhibited high CO oxidation activity with turnover frequency of 151 × 10−3 s−1 (1% CO balanced with air, atmospheric pressure, 27 °C). A systematical study of FeOx- and Al2O3-supported Pt, Pd catalysts by means of X-ray photoelectron spectroscopy, X-ray diffraction, high-resolution transmission electron microscopy, temperature-programmed reduction, H2–O2 titration, and time-resolved CO titration is reported. From 7% to 39% of Fe3+ was reduced to Fe2+ over Fe(OH)x-supported Pd and Pt catalysts, accompanied by Pd, Pt hydrogenation and hydroxyl loss, and a large amount of oxygen vacancies were proposed to be produced. Results of H2–O2 titration and time-resolved CO titration showed that a large amount of oxygen adsorbed onto FeOx support in the presence of Pt, Pd. This made CO oxidations over Pt/FeOx, Pd/FeOx proceed over two adjacent but different active sites (Pt, Pd for CO and FeOx for oxygen) with low apparent activation energies (30–34 kJ/mol), which accounted for their high activity in low-temperature CO oxidation.A Pt/FeOx catalyst exhibited high CO oxidation activity (TOF of 151 × 10−3 s−1, 1% CO balanced with air, atmospheric pressure, 27 °C) was reported. Clear evidence form characterizations show that FeOx acting as an oxygen supply is involved in the reaction.Download high-res image (132KB)Download full-size image
Co-reporter:Liguo Wang, Yubo Ma, Ying Wang, Shimin Liu, Youquan Deng
Catalysis Communications (15 September 2011) Volume 12(Issue 15) pp:1458-1462
Publication Date(Web):15 September 2011
DOI:10.1016/j.catcom.2011.05.027
Lanthanum oxide catalyst prepared by precipitation method and calcined at 600 °C exhibited better catalytic activity in the catalytic synthesis of glycerol carbonate from glycerol and urea with TOF up to 1506 mmol/g·h. It was proposed that the lanthanum oxide catalyst with more strong basic sites (Td > 400 °C) exhibited higher catalytic activity. Accordingly, the catalyst containing appropriate amount of La2O2CO3 phase exhibited higher catalytic activity. Moreover, the recycling experiments demonstrated that the catalytic activity can be essentially preserved during the recycling tests investigated.Lanthanum oxide catalyst prepared with precipitation method and calcined at 600 °C exhibited 89.1% of glycerol carbonate yield with 98.6% selectivity with as low as 1 wt.% catalyst amount in glycerolysis of urea, thereby leading to higher TOF of 1506 mmol/g·h as compared to the previous report.Download full-size imageResearch highlights► A series of rare earth oxides was tested in the carbonylation of glycerol with urea. ► Lanthanum oxide exhibited better catalytic activity in glycerol carbonate synthesis. ► The catalytic activity essentially correlated with the strong basicity (Td > 400 °C).
Co-reporter:Wenpeng Ni, Shimin Liu, Yuqing Fei, Yude He, Xiangyuan Ma, Liujin Lu, Youquan Deng
Journal of Electroanalytical Chemistry (15 February 2017) Volume 787() pp:
Publication Date(Web):15 February 2017
DOI:10.1016/j.jelechem.2017.01.056
•The oxidation of 1-methylimidazole in imidazolium-based ionic liquids was studied.•There are two oxidation peaks for the CV curves of 1-methylimidazole.•The limits of detection of 1-methylimidazole are about 20–35 ppm.•The effects of water and halide were researched.The voltammetric behaviors of room temperature ionic liquids (RTILs) are affected by many factors, including the structure of cation and anion, experimental conditions, impurities and so on. In this work, the determination of 1-methylimidazole (1-MIm) was explored in three imidazolium ionic liquids by virtue of cyclic voltammetry. On the anodic scans, the oxidation peaks of 1-MIm were observed for tested samples, and the linear correlation of the oxidation peak current against the concentration of 1-MIm could be established by standard addition method. The obtained results showed that the limits of detection reached 20–35 ppm while the limits of quantification were less than 100 ppm. Moreover, the influences of halide ions on the determination of 1-MIm in RTILs were also studied emphatically. It was found that the effect might arise from the reaction between 1-MIm and chlorine or bromine generated from the oxidation of Cl− or Br−, since the response of tri-halide was disappeared in the presence of 1-MIm according to the results of cyclic voltammetry and UV–Vis spectroscopy.
Co-reporter:Qinghua Zhang, Benqun Yang, Shiguo Zhang, Shimin Liu and Youquan Deng
Journal of Materials Chemistry A 2011 - vol. 21(Issue 41) pp:NaN16338-16338
Publication Date(Web):2011/09/20
DOI:10.1039/C1JM13828F
A new class of liquid fluorescent organic salts was designed and prepared through via a strategy of ionic liquidization. These new ionic liquid materials exhibited strong green fluorescence and remarkable solvent-dependent photoluminescence under UV irradiation. Their physicochemical properties, especially the fluorescent behaviour, were studied intensively.
Co-reporter:Shiguo Zhang, Yan Zhang, Ying Wang, Shimin Liu and Youquan Deng
Physical Chemistry Chemical Physics 2012 - vol. 14(Issue 15) pp:NaN5138-5138
Publication Date(Web):2012/02/13
DOI:10.1039/C2CP23675C
Ionic liquids (ILs)-stabilized iron oxide (Fe2O3) nanoparticles were synthesized by the ultrasonic decomposition of iron carbonyl precursors in [EMIm][BF4] without any stabilizing or capping agents. The Fe2O3 nanoparticles were isolated and characterized by X-ray powder diffraction, transmission electron microscopy and susceptibility measurements. The physicochemical properties of ILs containing magnetic Fe2O3 nanoparticles (denoted as Fe2O3@[EMIm][BF4]), including surface properties, density, viscosity and stability, were investigated in detail and compared with that of [EMIm][BF4]. The Fe2O3@[EMIm][BF4] can be directly used as magnetic ionic liquid marble by coating with hydrophobic and unreactive polytetrafluoroethylene (PTFE), for which the effective surface tension was determined by the puddle height method. The resulting magnetic ionic liquid marble can be transported under external magnetic actuation, without detachment of magnetic particles from the marble surface that is usually observed in water marble.
Co-reporter:Wenpeng Ni, Shimin Liu, Yuqing Fei, Yude He, Xiangyuan Ma, Liujin Lu and Youquan Deng
Journal of Materials Chemistry A 2016 - vol. 4(Issue 20) pp:NaN7753-7753
Publication Date(Web):2016/04/14
DOI:10.1039/C6TA01222A
The catalytic activity of a cathode material plays a vital role in determining the electrochemical performance of Li–O2 batteries. Herein, N-doped mesoporous carbon-supported CoO@Co nanoparticles are prepared in situ using the ionic liquid (IL) 1-butyl-3-methylimidazolium tetrachlorocobalt ([BMIm]2[CoCl4]) as the precursor with silica as the hard template. The material was characterized by TGA, BET, XRD, TEM, XPS, and H2-TPR. After exposure to air, the species on the surface of the Co is CoO, as verified by XPS. The pore size is about 2 nm, and the CoO@Co nanoparticles were irregularly shaped and sized in the range of 20–300 nm, which may have been due to the aggregation of ultrafine nanoparticles. The existence of an interaction between the CoO@Co nanoparticles and the N-doped support is confirmed by XPS and H2-TPR. The catalyst shows superior activity for oxygen evolution reaction (OER) manifested in its lower charge potential (3.75 V at the current density of 100 mA g−1). Enhanced performances in coulombic efficiency, rate capability, and cycling stability (55 cycles) are also realized. Finally, these improvements, with the exception of the catalytic activity of CoO, may benefit from the interaction between the carbon supporter and the CoO@Co nanoparticles.
Co-reporter:Shiguo Zhang, Shimin Liu, Qinghua Zhang and Youquan Deng
Chemical Communications 2011 - vol. 47(Issue 23) pp:NaN6643-6643
Publication Date(Web):2011/05/12
DOI:10.1039/C1CC11924A
A new class of azobenzene-based photoresponsive ionic liquids was prepared and showed reversible modulation of ionic conductivity in specific solvents under alternative UV/visible light irradiation.
Co-reporter:Zhengjian Chen, Shiguo Zhang, Xiujuan Qi, Shimin Liu, Qinghua Zhang and Youquan Deng
Journal of Materials Chemistry A 2011 - vol. 21(Issue 25) pp:NaN8982-8982
Publication Date(Web):2011/05/27
DOI:10.1039/C1JM11556A
Quinolizinium ionic liquids (salts) featuring an unbranched cation core have been prepared, characterized and found to show extremely high fluorescence quantum yields in solution (Φf > 99%, λem near 334 nm) and bright cyan fluorescence in molten state (λem near 465 nm).
Co-reporter:Qinghua Zhang, Xiangyuan Ma, Shimin Liu, Benqun Yang, Liujin Lu, Yude He and Youquan Deng
Journal of Materials Chemistry A 2011 - vol. 21(Issue 19) pp:NaN6868-6868
Publication Date(Web):2011/04/05
DOI:10.1039/C1JM10491H
Nine 1-allyl-3-alkylimidazolium ([ACnIm]) or 1-vinyl-3-alkylimidazolium ([VCnIm]) dicyanamides (DCA) were prepared and characterized, and their physicochemical properties were studied in detail. Except for [AVIm]DCA and [AC4Im]DCA, the other dicyanamides with hexyl or longer alkyl chains on the cation exhibited the characteristic of hydrophobicity. Among them, [AC8Im]DCA and [AC10Im]DCA were found to possess similar densities to water, i.e. 1.007 g cm−3 and 0.988 g cm−3 at 25 °C, respectively. Interestingly, a reversible phase reversion of a [AC8Im]DCA/H2O mixture was observed as the temperature varied. These environmentally-friendly liquid materials have potential applications as precursors for syntheses of conducting polymeric materials.
Co-reporter:Lequan Liu, Feng Zhou, Rajesh Kodiyath, Shigenori Ueda, Hideki Abe, Defa Wang, Youquan Deng and Jinhua Ye
Physical Chemistry Chemical Physics 2016 - vol. 18(Issue 42) pp:NaN29615-29615
Publication Date(Web):2016/10/04
DOI:10.1039/C6CP05289D
CO poisoning of Pt catalysts is one of the major challenges to the commercialization of proton exchange membrane fuel cells. One promising solution is to develop CO-tolerant Pt-based catalysts. A facilely synthesized Pt/FeOx catalyst exhibited outstanding CO tolerance in the oxidation of H2 and electrochemical CO stripping. Light-off temperature of H2O formation over Pt/FeOx was achieved even below 30 °C in the presence of 3000 ppm CO at a space velocity of 18000 mL g−1cat h−1. For the electrochemical oxidation of CO, the onset and peak potentials decreased by 0.17 V and 0.10 V, respectively, in comparison with those of commercial Pt/C. More importantly, by a combination of hard X-ray photoemission spectroscopy and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies it was found that the decreased electron density of Pt in Pt/FeOx enhanced the mobility of adsorbed CO, suppressed Pt–CO bonding and significantly increased the CO tolerance of Pt/FeOx.