Co-reporter:Jinli Zhang, Xian Wang, Yan Fu, You Han, Jingyao Cheng, Yanqing Zhang, and Wei Li
Langmuir November 26, 2013 Volume 29(Issue 47) pp:14345-14350
Publication Date(Web):August 14, 2013
DOI:10.1021/la402153b
Highly active subnano Pd clusters were synthesized using i-motif DNA as the template through characterization via ESI MS, DLS, XPS, UV–vis, and FTIR. It is indicated that Pd1–Pd5 clusters are generated at a [Pd]/[base] ratio of 0.2, Pd8 to Pd9 clusters are generated at a [Pd]/[base] ratio of 0.5, and large nanoparticles with the size about 2.6 nm are formed at a [Pd]/[base] ratio of 2.0. The i-motif-stabilized Pd8–Pd9 clusters show high catalytic activity toward the reduction of 4-nitrophenol with a relative rate constant value of 2034 min–1 (mM Pd)−1. DFT calculations disclose that the unique structure of the i-motif with consecutive hemiprotonated CH+·C pairs can efficiently ligate Pd ions at the N3 sites of cytosines and that the synthesized Pd clusters consist of metallic Pd atoms as well as positively charged Pd that is ligated by nucleobases, which is capable of facilitating the activation of the nitryl group of 4-nitrophenol. This work suggests a promising pathway to preparing subnano metal catalysts with enhanced catalytic activity using programmable DNA scaffolds.
Co-reporter:Shudan Zheng, You Han, Jinli Zhang, Wei Li
Fluid Phase Equilibria 2017 Volume 432() pp:18-27
Publication Date(Web):25 January 2017
DOI:10.1016/j.fluid.2016.10.021
The solubility data of linezolid form II in five pure solvents (water, methanol, ethanol, 1-propanol, 2-propanol) and a binary (water + methanol) solvent were determined among the temperature range from 283.15 K to 318.15 K under atmospheric pressure. The results indicated that the solubility increased with the temperature increasing. Seven thermodynamic models were used here to correlate the experimental solubility data. Through the comparison of the experimental data in pure solvents with the calculated results, we found that the modified Apelblat equation fit the experimental data best. Furthermore, the density functional theory (DFT) calculations showed that the solubility in different solvents related to the interaction strength between the linezolid and the solvent molecules. Finally, the molar enthalpy change, molar entropy change and molar Gibbs free energy change of dissolution of linezolid in the different solvents were also calculated by van't Hoff equation in this paper.
Co-reporter:Ying Feng;Junjie Gu;Feng Yu;Chunfu Lin;Jinli Zhang;Ning Nie
RSC Advances (2011-Present) 2017 vol. 7(Issue 53) pp:33544-33551
Publication Date(Web):2017/06/29
DOI:10.1039/C7RA04510G
A series of non-stoichiometric carbon-coated lithium iron phosphate (LiFexPO4/C) have been prepared by a solid-state reaction to study the variation of electrochemical performance at different x values. Characterized by XRD in conjunction with Rietveld refinement, Mössbauer, TEM, Raman, etc., it is indicated that the Li–O bond is elongated in the Fe-poor non-stoichiometric lithium iron phosphate with decreasing x value, while the content of Fe2P and graphitization degree of carbon layer in LiFexPO4/C samples is associated with the ratio of x. The powder electronic conductivity increases from 8.33 × 10−2 S cm−1 to 16.67 × 10−2 S cm−1 as the x value decreases from 1.04 to 0.98, which is due to a suitable amount of Fe2P and a superior graphitized carbon layer. Among different Fe/Li ratios, LiFe0.98PO4/C exhibits the highest rate capability of 163.5 mA h g−1 at 0.1C and 93.5 mA h g−1 at 20C, as well as the largest diffusion coefficient of 12.6 × 10−14 cm2 s−1. It is illustrated that the synergy effect of elongated Li–O bonds, moderate Fe2P and graphitized carbon layer results in the high performance of non-stoichiometric LiFexPO4/C.
Co-reporter:Wei Li, Chang Shi, Ayang Zhou, Xiao He, Yawei Sun, Jinli Zhang
Separation and Purification Technology 2017 Volume 186(Volume 186) pp:
Publication Date(Web):2 October 2017
DOI:10.1016/j.seppur.2017.05.044
•A positively charged NF membrane was synthesized via IP on the crosslinked polyetherimide.•EDTA was used for modification of the positively charged NF membrane.•A higher separation factor for LiCl/MgCl2was gotten after modification with EDTA.•The EDTA modified membrane shows stable performance for LiCl/MgCl2 separation.For efficient recovery of lithium from brines, a composite nanofiltration (NF) membrane with positively charged skin layer (PA-B) was first synthesized via interfacial polymerization between branched poly(ethylene imine) (BPEI) and trimesoyl chloride (TMC) on the support of crosslinked polyetherimide, and the separation performance was assessed for simulative brine of mixed LiCl/MgCl2 solution. To improve the permselectivity of Li+ against Mg2+, then we adopted EDTA to modify the as-prepared positively charged PA-B NF membrane. The optimal EDTA modified NF membrane PA-B2-E3 showed the separation factor SLi,Mg about 9.2 for the LiCl/MgCl2 mixed solution with a Mg2+/Li+ mass ratio of 24, with excellent stability within 36 h filtration, which would have promising applications in the recovery of Li from brine.
Co-reporter:Yuanyuan Liu, Junjie Gu, Jinli Zhang, Feng Yu, Lutao Dong, Ning Nie, Wei Li
Journal of Power Sources 2016 Volume 304() pp:42-50
Publication Date(Web):1 February 2016
DOI:10.1016/j.jpowsour.2015.11.022
•3D porous LFP/N-CNWs was synthesized using MIL-100(Fe) as template and raw material.•LFP/N-CNWs composite possess a high BET surface area of 129 m2 g−1.•LFP/N-CNWs shows excellent capacity and rate performance comparing with LFP/CNWs.Lithium iron phosphate (LiFePO4) nanoparticles embedded in the continuous interconnected nitrogen-doped carbon networks (LFP/N-CNWs) is an optimal architecture to fast electron and Li+ conduction. This paper, for the first time, reports a reasonable design and successful preparation of porous hierarchical LFP/N-CNWs composites using unique Fe-based metal organic framework (MIL-100(Fe)) as both template and starting material of Fe and C. Such nitrogen-doped carbon networks (N-CNWs) surrounding the lithium iron phosphate nanoparticles facilitate the transfer of Li+ and electrons throughout the electrodes, which significantly decreases the internal resistance for the electrodes and results in the efficient utilization of LiFePO4. The synthesized LFP/N-CNWs composites possess a porous structure with an amazing surface area of 129 m2 g−1, considerably enhanced electrical conductivities of 7.58 × 10−2 S cm−1 and Li+ diffusion coefficient of 8.82 × 10−14 cm2 s−1, thereby delivering excellent discharge capacities of 161.5 and 93.6 mAh·g−1 at 0.1C and 20C, respectively.
Co-reporter:Lijun Hou, Jinli Zhang, Yanfeng Pu and Wei Li
RSC Advances 2016 vol. 6(Issue 22) pp:18026-18032
Publication Date(Web):05 Feb 2016
DOI:10.1039/C5RA23112D
A series of N-doped spherical active carbons were synthesized via the pyrolysis of melamine in activated carbon, and used as a support to prepare Ru-based catalysts for an acetylene hydrochlorination reaction. The catalytic performance assessments indicate that the N-doped carbon support can increase greatly the activity and the stability of Ru-based catalysts. The optimal activity is achieved over Ru/SAC-N700, with an acetylene conversion of 99.8% under the conditions of 170 °C, C2H2 gas hour space velocity (GHSV) of 180 h−1, a feed volume ratio of V(HCl)/V(C2H2) of 1.1 after 30 h. Using characterizations of BET, FT-IR, XPS, TPR, TPD, TG, etc., it is illustrated that N-dopants can increase the dispersion of Ru elements, enhance the adsorption of reactants and the desorption of the product, and reduce significantly the coke deposition, consequently resulting in higher catalytic activity of Ru/SAC-N700. It is suggested that the pyridine–nitrogen plays an important role in augmenting the catalytic activity of Ru-supported catalysts.
Co-reporter:Jinli Zhang, Yuyan Hai, Yi Zuo, Qian Jiang, Chang Shi and Wei Li
Journal of Materials Chemistry A 2015 vol. 3(Issue 16) pp:8816-8824
Publication Date(Web):16 Mar 2015
DOI:10.1039/C4TA07159J
Novel polyamide thin film composite (TFC) nanofiltration (NF) membranes were prepared on polyetherimide supports by the interfacial polymerization of 1,2,4,5-benzene tetracarbonyl chloride and m-phenylenediamine followed by modification with ethylenediamine (EDA). The TFC NF membranes thus prepared were characterized by attenuated total reflection Fourier transform infrared (ATR-FTIR), solid-state nuclear magnetic resonance (NMR) and X-ray photoelectron spectroscopy (XPS); these results indicated that by covalent bonding with EDA, the unstable carboxylic groups on the initially generated poly(amic acid) (PAA) TFC membrane surfaces were effectively transformed into polyamide, including the methylene group in the chemical structure chain, for preparing the PAA-cov-EDA NF membranes. At an operating pressure of 1.0 MPa, the PAA-cov-EDA NF membrane exhibits a glucose rejection of 90% at a flux of 25 L m−2 h−1, and a MgSO4 rejection of 76% at a flux of 31 L m−2 h−1, in particular demonstrating its superior chlorine resistance, after being immersed in a 200 ppm NaClO solution for 100 h. Such novel polyamide TFC NF membranes have the advantages of mild preparation conditions and high rejection towards low-molecular-weight organics, thus demonstrating their potential in the pharmaceutical industry.
Co-reporter:Zhang Jinli, Wang Jiao, Liu Yuanyuan, Nie Ning, Gu Junjie, Yu Feng and Li Wei
Journal of Materials Chemistry A 2015 vol. 3(Issue 5) pp:2043-2049
Publication Date(Web):24 Nov 2014
DOI:10.1039/C4TA05186F
A novel composite of LiFePO4 with phosphorus-doped carbon layers has been prepared via a simple hydrothermal method using glucose as the carbon source to generate a carbon coating and triphenylphosphine as the phosphorus source. The effects of phosphorus doping on the phase purity, morphology and electrochemical performance of the materials are studied by the characterizations using X-ray diffraction, Raman spectroscopy, scanning electron microscopy, high resolution transmission electron microscopy and electrochemical techniques. It is indicated that phosphorus doping into the carbon layers is beneficial for the graphitization of the carbon. Phosphorus in the carbon layers exists in the form of P–C bonds and its concentration depends on the second calcination temperature. Moreover, the phosphorus-doped carbon layers on the particle surface make the charge transfer resistance decrease remarkably from 156.5 Ω to 49.1 Ω, which can be ascribed to the free carriers donated by phosphorus. The as-prepared LiFePO4 with phosphorus-doped carbon layers calcined at 600 °C shows the best electrochemical performance with a discharge capacity of 124.0 mA h g−1 at a high rate of 20 C and an excellent retention rate of 91.4% after 50 cycles. The LiFePO4 with phosphorus-doped carbon layers exhibits excellent electrochemical performances, especially at high current rates; thus, it is a promising cathode material for high-performance lithium ion batteries.
Co-reporter:Jinli Zhang, Ning Nie, Yuanyuan Liu, Jiao Wang, Feng Yu, Junjie Gu, and Wei Li
ACS Applied Materials & Interfaces 2015 Volume 7(Issue 36) pp:20134
Publication Date(Web):August 25, 2015
DOI:10.1021/acsami.5b05398
An evolutionary composite of LiFePO4 with nitrogen and boron codoped carbon layers was prepared by processing hydrothermal-synthesized LiFePO4. This novel codoping method is successfully applied to LiFePO4 for commercial use, and it achieved excellent electrochemical performance. The electrochemical performance can be improved through single nitrogen doping (LiFePO4/C–N) or boron doping (LiFePO4/C–B). When modifying the LiFePO4/C–B with nitrogen (to synthesis LiFePO4/C–B+N) the undesired nonconducting N–B configurations (190.1 and 397.9 eV) are generated. This decreases the electronic conductivity from 2.56 × 10–2 to 1.30 × 10–2 S cm–1 resulting in weak electrochemical performance. Nevertheless, using the opposite order to decorate LiFePO4/C–N with boron (to obtain LiFePO4/C–N+B) not only eliminates the nonconducting N–B impurity, but also promotes the conductive C–N (398.3, 400.3, and 401.1 eV) and C–B (189.5 eV) configurations—this markedly improves the electronic conductivity to 1.36 × 10–1 S cm–1. Meanwhile the positive doping strategy leads to synergistic electrochemical activity distinctly compared with single N- or B-doped materials (even much better than their sum capacity at 20 C). Moreover, due to the electron and hole-type carriers donated by nitrogen and boron atoms, the N+B codoped carbon coating tremendously enhances the electrochemical property: at the rate of 20 C, the codoped sample can elevate the discharge capacity of LFP/C from 101.1 mAh g–1 to 121.6 mAh g–1, and the codoped product based on commercial LiFePO4/C shows a discharge capacity of 78.4 mAh g–1 rather than 48.1 mAh g–1. Nevertheless, the B+N codoped sample decreases the discharge capacity of LFP/C from 101.1 mAh g–1 to 95.4 mAh g–1, while the commercial LFP/C changes from 48.1 mAh g–1 to 40.6 mAh g–1.Keywords: boron doping; carbon coating; electrochemical energy storage; lithium ion batteries; lithium iron phosphate; nitrogen doping
Co-reporter:Yuanyuan Liu, Junjie Gu, Jinli Zhang, Jiao Wang, Ning Nie, Yan Fu, Wei Li, Feng Yu
Electrochimica Acta 2015 Volume 173() pp:448-457
Publication Date(Web):10 August 2015
DOI:10.1016/j.electacta.2015.05.103
Decreasing particle size ensures a good accessibility for LiFePO4 to reach theoretical capacity and achieve high cycling rates owing to the improved Li-ion diffusion coefficient. In this paper, the size of LiFePO4 particle is successfully controlled hydrothermally through adjusting the size and morphology of its precursor precipitate via high shear mixer (HSM) without involving any environmentally toxic surfactants. It is indicated that the LiFePO4/C particles synthesized by HSM at the stirring rate of 1.3×104 rpm exhibit a reduced particle size of ∼220 nm and an enlarged surface area of 15.6 m2·g−1, which perform a high Li-ions diffusion coefficient of 1.43×10−13 cm2·s−1. The LiFePO4/C nanoparticles exhibit large discharge capacity of 160.1 mAh·g−1 at 0.1 C and even high rate capacity of 90.8 mAh·g−1 at 20 C. This work suggests that adjusting the size and morphology of the precursor precipitates is an effective way to quicken the nucleation and crystal growth, so that to obtain fine particles with high specific surface area and high crystalline purity.
Co-reporter:Yan Fu, Haixiang Zhang, Shengdong Dai, Xing Zhi, Jinli Zhang and Wei Li
Analyst 2015 vol. 140(Issue 19) pp:6676-6683
Publication Date(Web):03 Aug 2015
DOI:10.1039/C5AN01103E
Glutathione-capped Pd nanoparticles with a size of 1.4–3.5 nm are facilely synthesized for peroxidase nanomimetics. The molar ratio of [Na2PdCl4]/[GSH] greatly affects the physicochemical properties including particle sizes, surface charge states and enzymatic activities. The most efficient Pd-based nanozyme, consisting of approximately 57% metallic Pd0 species with an average diameter of 2.6 nm, exhibits the Km value of 0.068 mM toward 3,3′,5,5′-tetramethylbenzidine and 156 mM toward hydrogen peroxide. Ag+ selectively binds to Pd0 species through metallophilic interactions and induces an apparent aggregation of Pd nanoparticles. This is the first report that Ag+ significantly inhibits the peroxidase mimicking activity of Pd nanoparticles. A Pd-based nanozyme is employed to explore colorimetric detection of Ag+ with the limit of detection of 1.2 nM. This developed sensing system is potentially applicable for quantitative detection of Ag+ in drinking water as well as Ag nanoparticles in aqueous solution.
Co-reporter:Yuanyuan Liu, Junjie Gu, Jinli Zhang, Feng Yu, Jiao Wang, Ning Nie and Wei Li
RSC Advances 2015 vol. 5(Issue 13) pp:9745-9751
Publication Date(Web):05 Jan 2015
DOI:10.1039/C4RA14791J
Small grain size combined with large I(020)/I(111) ratio have been proven to be an effective strategy to improve the electrochemical properties of LiFePO4 material due to increased Li-ion diffusion. In view of this, we use Tween-80 as the surfactant in hydrothermal synthesis to modulate both crystal size and orientation of LiFePO4. It is indicated that the LiFePO4 particles synthesized via the Tween-80 modified hydrothermal method exhibited a small mean diameter of 100 nm and a large I(020)/I(111) ratio of 1.19. Whereas in the surfactant-free hydrothermal system, the obtained LiFePO4 particles exhibit a relatively large mean diameter of 200 nm and a low I(020)/I(111) ratio of 0.84. LiFePO4 particles with small grain size and a large I(020)/I(111) ratio can be easily brought into contact with electrolyte, facilitating electric and Li-ion diffusion. After being coated with conductive carbon, the synthesized LiFePO4/C nanoparticles perform a high Li-ion diffusion coefficient of 1.79 × 10−13 cm2 s−1. It presents a large reversible capacity of 166.5 mA h g−1 at 0.1 C and even a high rate capacity of 119.6 mA h g−1 at 20 C.
Co-reporter:Yunhe Jin, Guangbi Li, Jinli Zhang, Yanfeng Pu and Wei Li
RSC Advances 2015 vol. 5(Issue 47) pp:37774-37779
Publication Date(Web):14 Apr 2015
DOI:10.1039/C5RA03466C
Ruthenium and ruthenium–potassium bimetallic catalysts for acetylene hydrochlorination were prepared with RuCl3·H2O and KCl as precursors and active carbon as the support. It is found that Ru–K/SAC catalysts have a higher catalytic performance than Ru/SAC catalysts and the optimal conversion of acetylene over Ru1K1/SAC is 93.4% under the conditions of 170 °C, C2H2 hourly space velocity (GHSV) of 180 h−1, feed volume ratio V(HCl)/V(C2H2) = 1.1. Characterized with BET, TG, TEM, TPR, TPD and XPS, it is indicated that the K additive can promote the formation of more active RuO2 species during the catalyst preparation, but also enhance the ruthenium dispersion of catalysts. In particular, K additive can enhance the reactant adsorption and the product desorption properties of Ru-based catalysts, but also facilitate the function of auxiliary RuCl3 species to inhibit coke deposition.
Co-reporter:Wei Li, Liya Lou, Yuyan Hai, Changxin Fu and Jinli Zhang
RSC Advances 2015 vol. 5(Issue 67) pp:54125-54132
Publication Date(Web):10 Jun 2015
DOI:10.1039/C5RA02589C
Polyamide thin film composite nanofiltration membranes were synthesized on the polyethersulfone (PES) support via the interfacial polymerization between trimesoyl chloride (TMC) and the amine mixture of m-phenylenediamine (MPD) and thiourea (TU). It is indicated that the composite membrane (PES-M5T5) prepared at the MPD/TU ratio of 5:5 shows higher flux and glucose rejection than the membranes prepared using the individual amine. Further the optimal membrane PES-M5T5-TEA, prepared in the presence of triethylamine (TEA) additive, shows the largest flux of 39.7 L m−2 h−1 at an operation pressure of 1.6 MPa and the glucose rejection higher than 97.0%. In combination with characterizations of ATR-IR, Raman, SEM, XPS, AFM and contact angle measurements, it is illustrated that the TEA additive can promote the IP between TMC and MPD + TU, resulting in more amount of thioamide structures generated in the top layers of PES-M5T5-TEA, which can form more free volume and consequently improve the membrane flux. In addition, the PES-M5T5-TEA membrane shows excellent chlorine resistance against immersion of 200 ppm NaClO solution more than 100 h.
Co-reporter:Yan Fu;Xiongfei Chen;Jinli Zhang
Chirality 2015 Volume 27( Issue 4) pp:306-313
Publication Date(Web):
DOI:10.1002/chir.22430
Abstract
Natural polynucleotides including Micrococcus lysodeikticus and calf thymus DNA exhibit enantioselective recognition to S-ofloxacin regulated by Cu2+. This is the first report that ofloxacin and Cu2+ have cooperative effects on the local distortions of polynucleotides. At the [Cu2+]/[base] ratio of 0.1, S-ofloxacin is more liable to induce the locally distorted structures of polynucleotides, of which the association constant of S-ofloxacin toward DNA-Cu(II) is three times higher than that of the R-enantiomer. The apparent increase of adsorption capability and cooperativity, as well as the change of adsorption mechanism were detected in the adsorption of ofloxacin enantiomers on polynucleotides upon Cu(II)-coordination. This study not only discloses the effect of the chiral drug on the structural transition of long double-stranded DNA, but provides fundamental data to develop a novel enantioseparation method based on natural polynucleotides. Chirality 27:306-313, 2015. © 2015 Wiley Periodicals, Inc.
Co-reporter:Jiangjiexing Wu ; Li Huey Tan ; Kevin Hwang ; Hang Xing ; Peiwen Wu ; Wei Li ;Yi Lu
Journal of the American Chemical Society 2014 Volume 136(Issue 43) pp:15195-15202
Publication Date(Web):September 22, 2014
DOI:10.1021/ja506150s
A systematic investigation of the effects of different DNA sequences on the morphologies of silver nanoparticles (AgNPs) grown from Ag nanocube seeds is reported. The presence of 10-mer oligo-A, -T, and -C directed AgNPs growth from cubic seeds into edge-truncated octahedra of different truncation extents and truncated tetrahedral AgNPs, while AgNPs in the presence of oligo-G remained cubic. The shape and morphological evolution of the nanoparticle growth for each system is investigated using SEM and TEM and correlated with UV–vis absorption kinetic studies. In addition, the roles of oligo-C and oligo-G secondary structures in modulating the morphologies of AgNPs are elucidated, and the morphological evolution for each condition of AgNPs growth is proposed. The shapes were found to be highly dependent on the binding affinity of each of the bases and the DNA secondary structures, favoring the stabilization of the Ag{111} facet. The AgNPs synthesized through this method have morphologies and optical properties that can be varied by using different DNA sequences, while the DNA molecules on these AgNPs are also stable against glutathione. The AgNP functionalization can be realized in a one-step synthesis while retaining the biorecognition ability of the DNA, which allows for programmable assembly.
Co-reporter:Yanfeng Pu, Jinli Zhang, Xia Wang, Haiyang Zhang, Li Yu, Yanzhao Dong and Wei Li
Catalysis Science & Technology 2014 vol. 4(Issue 12) pp:4426-4432
Publication Date(Web):18 Jul 2014
DOI:10.1039/C4CY00769G
Gold and gold-based bimetallic catalysts for acetylene hydrochlorination were prepared with HAuCl4·4H2O and NiCl2·6H2O as precursors, and were analyzed with BET, TG, XRD, TEM, TPR, and XPS. The Au1Ni3/CSs catalyst shows both high activity and good stability, with a C2H2 conversion of 95.4% after 46 h under a gas hourly space velocity (GHSV) of C2H2 of 900 h−1. The results indicate that the addition of nickel to gold can inhibit the reduction of catalytically active Au3+ to Au0 and oxidize Au0 to Au+ during the preparation of Au-based/CSs catalysts, and weaken the occurrence of coke deposition on the catalyst surface, thus improving the stability of the catalyst.
Co-reporter:Baoguo Wang, Li Yu, Jinli Zhang, Yanfeng Pu, Haiyang Zhang and Wei Li
RSC Advances 2014 vol. 4(Issue 31) pp:15877-15885
Publication Date(Web):17 Mar 2014
DOI:10.1039/C4RA00478G
The phosphorus-doped carbon, consisting of phosphate groups in the surface, was prepared using triphenylphosphine as the phosphorus source and assessed as the support of Au catalysts for acetylene hydrochlorination reaction, characterized by FT-IR, XPS, Raman, TEM, BET, etc. This P-doped carbon support can enhance both the acetylene conversion and the selectivity to vinyl chloride monomer (VCM) over Au/SAC catalysts. Over the optimal Au/20% P-SAC-700 catalyst, the acetylene conversion is 99.9% and the selectivity to VCM equals 100% within 23 h of reaction. It is illustrated that the phosphorous groups in the P-doped carbon support, comprised of (PO4)3−and (PO3)−, can interact with the active gold species Au3+ and Au1+ so as to improve the dispersibility of catalytic active sites. And in the catalyst Au/20% P-SAC-700 the interactions of phosphorous groups (PO4)3−and (PO3)− can prevent the reduction of active gold species Au3+ and Au1+ into Au0, but also retard the coking deposition on the catalyst surface, suggesting that the modulation of phosphorus-dopants in the carbon supports is a promising route to explore efficient non-mercuric catalysts for PVC manufacture.
Co-reporter:Wei Li, Xiongfei Chen, Yan Fu, and Jinli Zhang and Wei Li
The Journal of Physical Chemistry B 2014 Volume 118(Issue 20) pp:5300-5309
Publication Date(Web):May 5, 2014
DOI:10.1021/jp412460y
The specific interactions of Cu2+ with self-complementary DNA sequences involving d[G4C4(GC)2G4C4], d[(GC)10], and d[(AT)10], as well as the chiral recognition mechanism of ofloxacin enantiomers via the CuII-modulated DNAs, were investigated using characterizations of circular dichroism, gel electrophoresis, FT-IR spectroscopy, UV melting measurement, electron paramagnetic resonance, and HPLC. The CuII-coordinated GC-rich DNAs exhibit amplified enantioselectivity toward the S-enantiomer of ofloxacin. Especially in the case of d[G4C4(GC)2G4C4], ofloxacin enantiomers intercalate into the two adjacent guanine bases through the minor groove mediated by Cu2+, which leads to a more favorable binding between S-ofloxacin and DNA. The highest ee value of ofloxacin enantiomers in the permeate after being adsorbed by the CuII–DNA complex is obtained as 49.2% in the R-enantiomer at the [Cu2+]/[base] molar ratio of 0.25, while at the [Cu2+]/[base] molar ratio of 0.05 the highest ee value of ofloxacin enantiomers in the retentate reaches 26.3% in the S-enantiomer. This work illustrates a novel promising route to construct DNA-based chiral selectors toward certain drug enantiomers through the programmable enantioselective recognition on the basis of DNA chirality and the specific binding of transition metal ions.
Co-reporter:Yan Fu ; Xuyin Zhao ; Jinli Zhang
The Journal of Physical Chemistry C 2014 Volume 118(Issue 31) pp:18116-18125
Publication Date(Web):July 10, 2014
DOI:10.1021/jp503242e
G-/C-rich oligonucleotides are chosen as the nucleation templates to synthesize Pt nanozymes with the size distribution of 1.7–2.9 nm, showing high activity to mimic peroxidase. The physicochemical properties including charge states and particle sizes are greatly associated with the DNA templates, the precursor ions as well as the molar ratios of [precursor]/[DNA]. As increasing the average size from 1.8 to 2.9 nm, the fraction of Pt0 species increases while the proportion of Pt2+ decreases. In the meanwhile, the Km value toward H2O2 decreases by three times, whereas toward TMB the Km increases by two times. The most efficient Pt nanozyme consisting of approximate 66% metallic Pt0 is stabilized by the i-motif RET2 with the average diameter of 2.9 nm. These results pave a promising way to manufacture metal nanozymes with facile modulation of physicochemical properties through programming DNA sequences.
Co-reporter:Yan Fu;Xiaoli Duan;Xiongfei Chen;Haixiang Zhang;Jinli Zhang
Chirality 2014 Volume 26( Issue 5) pp:249-254
Publication Date(Web):
DOI:10.1002/chir.22287
ABSTRACT
DNA-based chiral selectors are constructed to discriminate ofloxacin enantiomers through metal-ion anchoring on a special DNA double helix that contains successive GC pairs. The effects of metal ions involving Mg2+, Ni2+, Cu2+, Ag+, and Pt2+ were studied on the regulation of DNA chiral discrimination towards ofloxacin enantiomers. It is shown that DNA-Cu(II) complexes exhibit the highest enantioselectivities at the [Cu2+]/base ratio of 0.1. The enantiomeric excess can reach 59% in R-enantiomer after being adsorbed by the RET-Cu(II) complex. Stereoselective recognition of ofloxacin enantiomers on the double helix is tunable via external stimulus, providing a programmable desorption process to regenerate DNA. This DNA-based chiral selector exhibits excellent reusability without apparent loss of enantioselectivity after three cycles of adsorption and desorption. Chirality 26:249–254, 2014. © 2014 Wiley Periodicals, Inc.
Co-reporter:Yan Fu, Tiantian Huang, Bin Chen, Jue Shen, Xiaoli Duan, Jinli Zhang, Wei Li
Separation and Purification Technology 2013 Volume 107() pp:11-18
Publication Date(Web):2 April 2013
DOI:10.1016/j.seppur.2013.01.007
Bovine serum albumin (BSA) anchored on the surface of magnetic Fe3O4 nanoparticles (MNPs) were prepared using electrostatic adsorption and studied as a new magnetically chiral selector for the separation of chiral drug enantiomers. It is indicated that the immobilized BSA molecules on the magnetic nanoparticles using electrostatic adsorption retain their stereoselective recognition with site II-binding drug ibuprofen at pH 7.0 and site I-binding drug ofloxacin at pH 9.0, with a optimal loading of 467 mg BSA per gram of MNPs. For racemic ibuprofen and ofloxacin, single-stage adsorption gives an enantiomeric excess of 13% and 14%, and the multi-stage operation enhances the chiral performance providing the ee value of 54% and 39% respectively. As increasing the initial ee of enantiomeric mixtures, Δee levels of 50%, 35% and 16% for stronger binder ibuprofen, as well as 31%, 17% and 13% for weaker binder ofloxacin are achieved under the same operational conditions. Depending upon the eutectic point of racemic compound, a hybrid process involving the enrichment of one enantiomer using BSA–PDDA–MNPs followed by subsequent crystallization is proposed to obtain the enantiomer with higher optical purity.Graphical abstractHighlights► BSA modified magnetic nanoparticles are utilized as novel chiral selectors. ► Immobilized BSA exhibit chiral discrimination for ibuprofen and ofloxacin. ► Multi-stage adsorption significantly enhances the enantiomeric excess. ► A hybrid resolution approach is proposed to obtain pure enantiomers.
Co-reporter:J. Zhang;Z. Feng;X. Jia;S. Xu;W. Li;M. Du
Chemical Engineering & Technology 2013 Volume 36( Issue 2) pp:241-250
Publication Date(Web):
DOI:10.1002/ceat.201200491
Abstract
The hydrodynamic, heat and mass transfer characteristics of a pressurized co-current gas-solid magnetically fluidized bed (MFB) were systematically investigated considering major influence factors, such as magnetic field strength, superficial gas velocity, and operating pressure. It was shown that this pressurized gas-solid MFB has the advantages of a wider operation range of the superficial gas velocity under bubble-free particulate fluidization, a larger bed voidage with smaller pressure drop across the bed, and larger heat transfer efficiency, compared with a conventional fluidized bed. Moreover, the minimum bubbling velocity, gas-solid mass, and heat transfer coefficients were correlated at high accuracy within the investigated range of operating conditions.
Co-reporter:Wei Li, Lu Liu, Yan Fu, Yanhua Sun, Jinli Zhang and Rongxin Zhang
Photochemical & Photobiological Sciences 2013 vol. 12(Issue 10) pp:1864-1872
Publication Date(Web):22 Jul 2013
DOI:10.1039/C3PP50026H
Silver nanoclusters (Ag NCs) with emission wavelengths from 538 nm to 706 nm were synthesized using a series of G-/C-rich polymorphic DNA templates. Thermodynamic studies on the interactions of Ag+ with polymorphic DNA indicate that the binding affinities greatly depend on the secondary structures of DNA templates, with a decreasing order: the coiled C-rich strand > the i-motif > the duplex > the G-quadruplex. Fluorescent Ag NCs prepared using these polymorphic DNA templates show that fluorescence stabilities are associated with the binding affinities between DNA templates and Ag+, e.g., the coiled C-rich strand C4A4C3 with the highest binding constant (40.2 × 105 M−1) stabilizes Ag NCs for over 300 h, while the G-quadruplex G4T4G4 with the lowest binding constant (0.64 × 105 M−1) generates Ag NCs with the shortest shelf-life (55 h). The cluster sizes of Ag NCs are associated with the sequence lengths of DNA templates. In addition, the red emitting [C4A4C3]-Ag and the NIR emitting [G4T4G4-C4A4C4]-Ag are successfully used for HeLa cell transfection and exhibit good intracellular emission. These results provide a promising pathway to prepare silver nanomaterials with desirable physicochemical properties through designing suitable DNA templates.
Co-reporter:Wei Li;Yingming Fu;Yan Fu;Xian Wang;Jinli Zhang
Catalysis Letters 2013 Volume 143( Issue 6) pp:578-586
Publication Date(Web):2013 June
DOI:10.1007/s10562-013-0989-3
Pd nanoparticles with narrow size distributions between 1.3 and 3.3 nm are prepared using G-/C-rich oligonucleotide as the template. These DNA-Pd nanoparticles efficiently catalyze the Suzuki coupling reaction and exhibit highly catalytic activities under mild conditions, which are greatly dependent upon the particle size of Pd nanoparticles besides the DNA sequence. For the coupling reaction of iodobenzene and phenylboronic acid at 60 °C in the presence of KOH, it can be achieved high TOF value of 2646 mol biphenyl (mol Pd × h)−1 over AG22-Pd and 3640 mol biphenyl (mol Pd × h)−1 over CT22-Pd. Under the optimal experimental conditions, the yield of 100 % in biphenyl is obtained with only 0.0055 mol% AG22-Pd at 60 °C for 1 h in the solvent of EtOH/H2O (1:2) using Na2CO3 or K2CO3 as the base. It is illustrated that G-/C-rich oligonucleotides are promising templates to modulate easily the morphology of Pd nanoparticles in aqueous solution with high catalytic activity.
Co-reporter:Jinli Zhang, Xian Wang, Yan Fu, You Han, Jingyao Cheng, Yanqing Zhang, and Wei Li
Langmuir 2013 Volume 29(Issue 47) pp:14345-14350
Publication Date(Web):August 14, 2013
DOI:10.1021/la402153b
Highly active subnano Pd clusters were synthesized using i-motif DNA as the template through characterization via ESI MS, DLS, XPS, UV–vis, and FTIR. It is indicated that Pd1–Pd5 clusters are generated at a [Pd]/[base] ratio of 0.2, Pd8 to Pd9 clusters are generated at a [Pd]/[base] ratio of 0.5, and large nanoparticles with the size about 2.6 nm are formed at a [Pd]/[base] ratio of 2.0. The i-motif-stabilized Pd8–Pd9 clusters show high catalytic activity toward the reduction of 4-nitrophenol with a relative rate constant value of 2034 min–1 (mM Pd)−1. DFT calculations disclose that the unique structure of the i-motif with consecutive hemiprotonated CH+·C pairs can efficiently ligate Pd ions at the N3 sites of cytosines and that the synthesized Pd clusters consist of metallic Pd atoms as well as positively charged Pd that is ligated by nucleobases, which is capable of facilitating the activation of the nitryl group of 4-nitrophenol. This work suggests a promising pathway to preparing subnano metal catalysts with enhanced catalytic activity using programmable DNA scaffolds.
Co-reporter:Wei Li;Yanli Li;Yan Fu;Jinli Zhang
Korean Journal of Chemical Engineering 2013 Volume 30( Issue 7) pp:1448-1453
Publication Date(Web):2013 July
DOI:10.1007/s11814-013-0048-1
Natural biomacromolecules including bovine serum albumin (BSA), calf thymus DNA (ct-DNA) and fish sperm DNA (fs-DNA) were studied as the free chiral selectors to separate R- and S-ofloxacin enantiomers from racemic ofloxacin, combined with ultrafiltration and subsequent crystallization. First, the interactions between chiral ofloxacin and biomacromolecules including BSA, ct-DNA, and fs-DNA were investigated using circular dichroism and fluorescence spectroscopy. BSA exhibited stereoselective adsorption towards R-ofloxacin at pH 9.0 with an enantioselectivity of 1.23, while ct-DNA showed enantiospecific interaction with S-enantiomer with the selectivity of 1.70 at pH 5.0. One single-stage adsorption by BSA provides an enantiomeric excess in the permeate (e.e.p) of 14% in S-enantiomer, and five-stage operations enhance the chiral resolution to reach the e.e.p value of 44%. R-enantiomer with an e.e.p of −26% can be obtained through one single-stage adsorption by using ct-DNA, and −85% can be reached by five-stage operations. Enantiomeric mixtures with the intial e.e. of 44% (S-) can be upgraded to 95% (S-) through subsequent crystallization. This programmable process of adsorption and desorption using BSA or ct-DNA as chiral selectors can be successfully applied to produce the enantiomers with highly optical purity.
Co-reporter:Jiangjiexing Wu, Yan Fu, Zhenghua He, You Han, Lin Zheng, Jinli Zhang, and Wei Li
The Journal of Physical Chemistry B 2012 Volume 116(Issue 5) pp:1655-1665
Publication Date(Web):January 13, 2012
DOI:10.1021/jp206251v
The aggregation behaviors of silver atoms modulated by polymorphic DNA templates involving i-motif, G-quadruplex, and the Watson–Crick duplex, were investigated by using the density functional theory (DFT) calculations, combining with the experimental characterizations of CD, UV, fluorescence measurements and TEM, in order to understand the reason in the molecular level that polymorphic DNA templates affect the fluorescence emitting species of Ag nanomaterials. First, the affinity sites of silver ions on different DNA templates were analyzed by using DFT calculations, and the conformational variations of DNA templates caused by silver ions and atoms were disclosed. Second, the aggregation behaviors of silver atoms constrained by the polymorphic DNA templates were studied by DFT modeling, and distinct fluorescence property of nanosilvers templated by polymorphic DNA were evaluated using the time-dependent DFT calculations. It is illustrated that with the DNA template adopting i-motif or the duplex the silver atoms tend to aggregate inside the encapsulated spaces of nucleobases, and the formed silver nanoclusters are positively charged with high fluorescent spectral features; whereas with the template of the G-quadruplex the silver atoms are preferential to aggregate outside of the G-tetrad, which results in the formation of larger silver crystals without fluorescence property. The results obtained here are useful to explore the nucleation and growth mechanism of silver nanomaterials regulated by the structure-specific DNA templates, which is important to rational design of desirable fluorescent emitters for sensing in the field from biology to nanoscience.
Co-reporter:Jinli Zhang, Anyuan Liu, You Han, Yan Ren, Junbo Gong, Wei Li, and Jingkang Wang
Crystal Growth & Design 2011 Volume 11(Issue 12) pp:5498-5506
Publication Date(Web):November 3, 2011
DOI:10.1021/cg201083r
Selective crystallization of tolbutamide on SAMs with the similar molecule structure of tolbutamide and the functional groups of methyl, trifluoromethyl, and phenyl respectively was studied through characterizations of XRD and crystal morphologies. It is indicated that at low supersaturation tolbutamide (TB) crystallized into form II on the methyl-terminated SAMs and trifluoromethyl-terminated SAMs, whereas the highest bioavailable TB crystals of form IV were obtained on phenyl-terminated SAMs, differing from the precipitated crystals from the solution including TB forms I, II, and III together. The preferential growth orders of the crystallographically important faces of TB forms I–IV were assessed on different functionalized SAMs through molecular modeling based on the prediction of equilibrium morphologies of crystals, which is in accordance with the experimental results. Further time-resolved Raman spectra of TB crystals grown on phenyl-terminated SAMs illustrate that the surface functional groups are paramount to adjust the heterogeneous nucleation of tolbutamide polymorphs at low supersaturation. This work provides a feasible approach combining the experimental with molecular modeling methods to understand deeply the relationship between interfacial functional groups of SAMs and molecular packing of crystals, which is fundamental to the rational design of experimental work on selective crystallization of organic crystals.
Co-reporter:Yan Fu, Xian Wang, Jinli Zhang, Ying Xiao, Wei Li, and Jingkang Wang
Biomacromolecules 2011 Volume 12(Issue 3) pp:
Publication Date(Web):January 14, 2011
DOI:10.1021/bm101372h
Spermine-induced orderly assembling properties of G-/C-rich oligonucleotides are investigated in dilute and crowding conditions. The first time we report that the parallel G-quadruplexes is preferential to condense into anisotropic microaggregates in the presence of spermine, whereas the hybrid-type and the antiparallel G-quadruplexes have no significant interactions with spermine; and spermine can induce the condensation of i-motif C-rich oligonucleotides other than the random coiled C-rich strands. Moreover, the condensation of C-rich oligonucleotides can be reversibly regulated by pH and temperature. G-/C-rich oligonucleotides exhibit the cholesteric liquid crystalline phase at low strand concentration in the presence of spermine under crowding conditions. The results illuminate that the parallel G-quadruplex and i-motifs are probably necessity conformations for G-/C-rich oligonucleotides that involved in the regulation of chromosome organization in living cells.
Co-reporter:Yan Fu ; Jinli Zhang ; Xiongfei Chen ; Tiantian Huang ; Xiaoli Duan ; Wei Li ;Jingkang Wang
The Journal of Physical Chemistry C 2011 Volume 115(Issue 21) pp:10370-10379
Publication Date(Web):May 6, 2011
DOI:10.1021/jp200132b
Silver nanomaterials with distinct fluorescent properties are synthesized with a series of G-rich/C-rich DNA templates, and the influence of DNA conformational structures on the size and the fluorescence of silver nanomaterials was investigated through varying the sequence composition and the ratio of complementary sequences, using CD, UV–vis, fluorescence spectroscopy, and TEM. It is intriguing to find out that G-rich templates at acidic conditions are capable of generating red emitters that are susceptible to the G-quadruplex structures associated with the number of 5′-terminal guanines. C-rich sequences can produce red silver clusters at either acidic or neutral conditions, and the emission is dramatically regulated by the number of 3′-end cytosines. It is the first time to report that double-stranded DNA templates can generate distinct fluorescent nanosilver modulated by the predominance among the structural competition of the Watson–Crick duplex, G-quadruplex, and i-motif. These results provide a promising pathway to prepare silver nanomaterials with desirable physicochemical properties through designing suitable DNA templates.
Co-reporter:Jinli Zhang, Lijuan Wang, Dan Wang, Junbo Gong, Wei Li, and Jingkang Wang
Journal of Chemical & Engineering Data 2011 Volume 56(Issue 3) pp:671-673
Publication Date(Web):February 14, 2011
DOI:10.1021/je101165m
The solubility of dexibuprofen in ethanol, n-propanol, isopropyl alcohol, ethyl acetate, and n-hexane was measured in the temperature range between (263.15 and 293.15) K under atmospheric pressure. The results indicated that the solubility of dexibuprofen in the selected solvents increased with increasing temperature. The experimental data were correlated by the modified Apelblat model.
Co-reporter:Lin Zheng;Ruichao Zhang;Yuxiang Ni;Qian Du;Xian Wang;Jinli Zhang
Catalysis Letters 2010 Volume 139( Issue 3-4) pp:145-150
Publication Date(Web):2010 November
DOI:10.1007/s10562-010-0419-8
This study describes the synthesis of Ag nanoparticles using DNA templates with polymorphic structures including the G-quadruplex, the I-motif, and the Duplex and their application for the catalytic reduction of 4-nitrophenol by NaBH4. Interactions between Ag+ and polymorphic DNA were studied through circular dichroism, polyacrylamide gels, and UV spectroscopy. Ag nanoparticles with narrow size distributions were prepared through the reduction of Ag+ by NaBH4 under different DNA templates and Ag+/base ratios. These DNA-templated Ag nanoparticles demonstrated excellent catalytic performance in the reduction reaction of 4-nitrophenol. The rate constants depended on the structure of DNA template, with the decreasing order: I-motif-Ag > G-quadruplex-Ag > Duplex-Ag. The results obtained here suggest a promising pathway to adjust physical–chemical properties of metal nanoparticles through the template of polymorphic DNA.
Co-reporter:Jinli Zhang, Lin Zheng, Xian Wang, Ying Xiao, Yi Lu, Wei Li
Materials Research Bulletin 2010 45(12) pp: 1954-1959
Publication Date(Web):
DOI:10.1016/j.materresbull.2010.08.008
Co-reporter:Zhijian Chen
Frontiers of Chemical Science and Engineering 2010 Volume 4( Issue 1) pp:1
Publication Date(Web):2010 March
DOI:10.1007/s11705-009-0306-2
Co-reporter:Daqing Li;Hao Li;Yan Fu;Jin-Li Zhang;Yong-Cai Han;Li Wang
Colloid Journal 2008 Volume 70( Issue 6) pp:747-752
Publication Date(Web):2008 December
DOI:10.1134/S1061933X08060100
The influence of micelle morphology transformation on the structure of mesoporous materials is fundamental in designing optimal, well-ordered, mesoporous materials. Firstly, the steady-state fluorescence technique was adopted to determine the first and second critical micelle concentrations of cetyltrimethylammonium chloride (CTAC) as 125 and 210 mmol L−1 in an equimolar mixture of water and ethanol at 25°C. Using tetraethylorthosilicate (TEOS) as the precursor, mesoporous silicas (with a surface area of 545.7–1210.5 m 545.7 ∼ 1210.5 m2 g−1 and a pore volume of 0.26 ∼ 0.80 cm3 g−1) were synthesized with the CTAC templates in the equimolar mixture of water and ethanol. Characterization by small-angle X-ray diffraction and N 2 adsorption/desorption techniques revealed that the surface area and pore volume of silica increased with the content of CTAC, whereas there existed a transition point at the CTAC/TEOS ratio of 0.15 corresponding to the fade-away of well-ordered mesoporous structure. The negative effect of the much higher content CTAC on the periodic structure of mesoporous silica is attributed to micelle transformation from spheres to cylinders related to the second critical micelle concentration of CTAC.
Co-reporter:Jin-Li Zhang, Wei Li, Xiang-Kun Meng, Li Wang, Li Zhu
Journal of Membrane Science 2003 Volume 222(1–2) pp:219-224
Publication Date(Web):1 September 2003
DOI:10.1016/S0376-7388(03)00292-8
The mesoporous silica/alumina membrane was prepared by the template-tailored sol–gel method, using the surfactant of cetyltrimethyl ammonium bromide (CTAB) as the template. Further a novel procedure was explored to synthesize free-standing mesoporous silica oriented by the self-assembles of surfactants. Characterization of SEM and BET indicated that this free-standing silica films had good development of mesoporosity and a special asymmetric structure, which make it not only an attractive materials for preparing new types of catalysts, medical carriers and chemical sensors, etc. but also has promising applications in manufacturing asymmetric mesoporous membranes.
Co-reporter:Yanfeng Pu, Jinli Zhang, Li Yu, Yunhe Jin, Wei Li
Applied Catalysis A: General (November 2014) Volume 488() pp:28-36
Publication Date(Web):November 2014
DOI:10.1016/j.apcata.2014.09.037
Co-reporter:Yan Fu, Jinjin Yang, Jinli Zhang, Wei Li
Chinese Journal of Chemical Engineering (January 2016) Volume 24(Issue 1) pp:31-38
Publication Date(Web):1 January 2016
DOI:10.1016/j.cjche.2015.07.003
Biomacromolecules including protein and nucleic acids are considered as promising chiral selectors in the fields of enantioselective separation, owing to their inherent chirality, polymorphous structures, stable physicochemical properties, good biocompatibility as well as susceptible modification and regulation. In this review, firstly, enantioselective recognition mechanism of proteins and nucleic acids toward different enantiomers is discussed, as well as their potential applications on the chiral separation of racemic compounds. Secondly, preparative enantioseparation adopting biomolecule-modified hybrid materials including porous microspheres, magnetic nanoparticles and affinity membranes, are introduced respectively. Finally, novel chiroptical materials constructed on the basis of chiral induction, transfer, amplification and transcription, are recognized as promising candidates in future applications.
Co-reporter:Yan Fu, Xian Wang, Jinli Zhang, Wei Li
Current Opinion in Biotechnology (August 2014) Volume 28() pp:33-38
Publication Date(Web):1 August 2014
DOI:10.1016/j.copbio.2013.10.014
•Switchable nanomachines and responsive nanomaterials.•Nano/subnano metal clusters with desirable physicochemical properties.•Chiral selectors and asymmetric catalysts.Besides the inherent chirality, DNA is enriched by nitrogen and oxygen functional groups that are preferential to coordinate with transition metal ions, and its self-assembled structures, including the G-quadruplex, the i-motif, and the conventional Watson–Crick duplex, etc., can be adjusted via different base pairings. Recently biotemplating on the basis of DNA self-assembly has been considered as an attractive method to construct switchable nanomaterials, to direct crystal growth and to design enantioselective selectors/catalysts. This review briefly covers the recent progress relevant to DNA modulated nano/subnano materials. The long-term goal of this area of research is to explore novel promisingly environmental-benign approaches to construct switchable nanomachines, nano/subnano clusters and enantioselective recognition platforms respectively, through DNA-based modulation.Download high-res image (286KB)Download full-size image
Co-reporter:Xiaoyan Li, Jinli Zhang, Wei Li
Journal of Industrial and Engineering Chemistry (25 December 2016) Volume 44() pp:146-154
Publication Date(Web):25 December 2016
DOI:10.1016/j.jiec.2016.08.024
A series of ZIF-derived nitrogen-doped carbon materials were prepared using melamine as the additional nitrogen sources for acetylene hydrochlorination. The results indicated that the optimal complex of Z4M1 exhibits the highest acetylene conversion of 60% under the reaction conditions of 180 °C, C2H2 gas hourly space velocity (GHSV) = 50 h−1, VHCl/VC2H2 = 1.15, suggesting a promising metal-free catalyst for acetylene hydrochlorination. It is illustrated that the additions of melamine not only make the complex of Z4M1 displays special morphological structure and proper pore structure, but also adjust the relative content ratio of three nitrogen species in ZIF-derived nitrogen-doped carbon materials.
Co-reporter:Baoguo Wang, Lijuan Wang, Jinli Zhang, Wei Li, Jingkang Wang
Thermochimica Acta (20 July 2012) Volume 540() pp:
Publication Date(Web):20 July 2012
DOI:10.1016/j.tca.2012.04.016
The solubilities of dexibuprofen in five solvents including methanol, n-butyl alcohol, isobutyl alcohol, n-amyl alcohol, and n-octyl alcohol were measured in the temperature range 263.15–293.15 K under atmospheric pressure. The results indicate that the solubilities of dexibuprofen in the selected solvents increase with temperature. The experimental data were correlated by the modified Apelblat model which fit well with the experimental data. The dissolution enthalpy and entropy of both rac-ibuprofen and dexibuprofen were predicted. Moreover, the solubility data of both of them were correlated using two local composition models: NRTL 1 and UNIQUAC. It is indicated that for dexibuprofen, the NRTL 1 model can provide more accurate estimations of the solubility in the solvents of methanol, ethanol and n-propyl alcohol, while both NRTL 1 and UNIQUAC models can provide good estimations of the solubility in other solvents. For the rac-ibuprofen, the UNIQUAC model performs better to estimate the solubility in all the solvents.Highlights► We measured the solubility data and correlated them by the modified Apelblat model. ► The dissolution enthalpy and entropy of both rac-ibuprofen and dexibuprofen were predicted. ► The solubility data were correlated using NRTL 1 and UNIQUAC model. ► The ΔHd, ΔSd and ΔGd values were estimated and analyzed. ► We made the distinctions between the models for the (S)-enantiomer and the racemate.
Co-reporter:Yanfeng Pu, Jinli Zhang, Xia Wang, Haiyang Zhang, Li Yu, Yanzhao Dong and Wei Li
Catalysis Science & Technology (2011-Present) 2014 - vol. 4(Issue 12) pp:NaN4432-4432
Publication Date(Web):2014/07/18
DOI:10.1039/C4CY00769G
Gold and gold-based bimetallic catalysts for acetylene hydrochlorination were prepared with HAuCl4·4H2O and NiCl2·6H2O as precursors, and were analyzed with BET, TG, XRD, TEM, TPR, and XPS. The Au1Ni3/CSs catalyst shows both high activity and good stability, with a C2H2 conversion of 95.4% after 46 h under a gas hourly space velocity (GHSV) of C2H2 of 900 h−1. The results indicate that the addition of nickel to gold can inhibit the reduction of catalytically active Au3+ to Au0 and oxidize Au0 to Au+ during the preparation of Au-based/CSs catalysts, and weaken the occurrence of coke deposition on the catalyst surface, thus improving the stability of the catalyst.
Co-reporter:Jinli Zhang, Yuyan Hai, Yi Zuo, Qian Jiang, Chang Shi and Wei Li
Journal of Materials Chemistry A 2015 - vol. 3(Issue 16) pp:NaN8824-8824
Publication Date(Web):2015/03/16
DOI:10.1039/C4TA07159J
Novel polyamide thin film composite (TFC) nanofiltration (NF) membranes were prepared on polyetherimide supports by the interfacial polymerization of 1,2,4,5-benzene tetracarbonyl chloride and m-phenylenediamine followed by modification with ethylenediamine (EDA). The TFC NF membranes thus prepared were characterized by attenuated total reflection Fourier transform infrared (ATR-FTIR), solid-state nuclear magnetic resonance (NMR) and X-ray photoelectron spectroscopy (XPS); these results indicated that by covalent bonding with EDA, the unstable carboxylic groups on the initially generated poly(amic acid) (PAA) TFC membrane surfaces were effectively transformed into polyamide, including the methylene group in the chemical structure chain, for preparing the PAA-cov-EDA NF membranes. At an operating pressure of 1.0 MPa, the PAA-cov-EDA NF membrane exhibits a glucose rejection of 90% at a flux of 25 L m−2 h−1, and a MgSO4 rejection of 76% at a flux of 31 L m−2 h−1, in particular demonstrating its superior chlorine resistance, after being immersed in a 200 ppm NaClO solution for 100 h. Such novel polyamide TFC NF membranes have the advantages of mild preparation conditions and high rejection towards low-molecular-weight organics, thus demonstrating their potential in the pharmaceutical industry.
Co-reporter:Zhang Jinli, Wang Jiao, Liu Yuanyuan, Nie Ning, Gu Junjie, Yu Feng and Li Wei
Journal of Materials Chemistry A 2015 - vol. 3(Issue 5) pp:NaN2049-2049
Publication Date(Web):2014/11/24
DOI:10.1039/C4TA05186F
A novel composite of LiFePO4 with phosphorus-doped carbon layers has been prepared via a simple hydrothermal method using glucose as the carbon source to generate a carbon coating and triphenylphosphine as the phosphorus source. The effects of phosphorus doping on the phase purity, morphology and electrochemical performance of the materials are studied by the characterizations using X-ray diffraction, Raman spectroscopy, scanning electron microscopy, high resolution transmission electron microscopy and electrochemical techniques. It is indicated that phosphorus doping into the carbon layers is beneficial for the graphitization of the carbon. Phosphorus in the carbon layers exists in the form of P–C bonds and its concentration depends on the second calcination temperature. Moreover, the phosphorus-doped carbon layers on the particle surface make the charge transfer resistance decrease remarkably from 156.5 Ω to 49.1 Ω, which can be ascribed to the free carriers donated by phosphorus. The as-prepared LiFePO4 with phosphorus-doped carbon layers calcined at 600 °C shows the best electrochemical performance with a discharge capacity of 124.0 mA h g−1 at a high rate of 20 C and an excellent retention rate of 91.4% after 50 cycles. The LiFePO4 with phosphorus-doped carbon layers exhibits excellent electrochemical performances, especially at high current rates; thus, it is a promising cathode material for high-performance lithium ion batteries.
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