Energy Storage Materials
·
2021
·
IF 17.789
Chao Yue Zhang,Guo Wen Sun,Zu De Shi,Qian Yu Liu,Jiang Long Pan,Yan Chun Wang,Hao Zhao,Geng Zhi Sun,Xiu Ping Gao,Xiao Jun Pan,Jin Yuan Zhou
Atom-intercalated transition metal disulfides (TMDs) have attached much attention mainly due to their highly improved conductivity. But it is few reported that the atom intercalation can enable the TMDs have unexpected catalytic properties, caused by the unit-cell deformation in them. In this work, a type of V 0.25 -intercalated VS 2 (V 5 S 8 ) nanoflakes was designed via a direct vulcanization method combining Kirkendall heat diffusion effect, and used as the promotor for lithium-sulfur batteries (LSBs). The V 5 S 8 possesses a NiAs crystal structure, in which V atoms occupy the interlayer spacing between VS 2 monolayers, which will unavoidably cause the unit-cell deformation. As expected, the CNF@V 5 S 8 /S cathodes show a specific capacity of 1260 mAh g −1 at 0.2 C, and can keep 73.65% of the capacity with charge/discharge rate increasing 10 times; while the CNF@VS 2 /S ones can only retain 54.0% of the initial capacity. Moreover, the CNF@V 5 S 8 /S cathodes show an ultralow decay rate of only 0.0312% per cycle for 1500 cycles at 5 C. Furthermore, the catalysis effect of V 5 S 8 on the conversion of lithium polysulfide (Li 2 S n , n = 1, 2, 4, 6 and 8) and S 8 clusters were systematically discusses. Besides, the V 5 S 8 can further enable LSBs achieve a high areal capacity (8.2 mAh cm −2 with sulfur loading of 7.8 mg cm −2 ) and a high dynamic flexible stability at bending angle between 0 and 180 °.
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高影响因子
GREEN CHEMISTRY
·
2021
·Vol. 23
·期 21
·8571-8580
·
IF 10.182
Yuting He,Huimin Lu,Xue Li,Jun Wu,Tiancheng Pu,Wei Du,Hongping Li,Jing Ding,Hui Wan,Guofeng Guan
The multi-step reaction of CO2 over basic catalysts significantly improves the diversity of products, vividly embodying the ability of green chemistry to turn waste into treasure. However, under a Lewis acidic CO2 atmosphere, the activity maintenance of the multi-step reaction puts forward higher requirements for the reversible regeneration ability of the basic catalysts. Novel Lewis–Brønsted binary basic poly(ionic liquid)s (LB-PILs) were successfully developed through a radical copolymerization followed by ion-exchange strategy, and were applied to the two-step synthesis of dimethyl carbonate (DMC) by coupling CO2 cycloaddition and CH3OH transesterification without any cocatalyst. Relying on the activation of CO2 by Lewis basic tertiary N and the thermal recovery of nucleophilic HCO3− to stronger Brønsted basic OH− with the help of temperature control in CH3OH transesterification, the LB-PILs presented high activity, stable repeatability and linear carbonate universality. In situ IR analysis and Knoevenagel condensation, combined with theoretical calculations, provided reliable support for the ingenious incorporation of reversible regeneration of basic catalysts in a Lewis acidic CO2 atmosphere and multi-step coupling reaction process of CO2.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Mengwei Guo,Zhuoming Wei,Qibo Zhang
The rational design and synthesis of highly efficient, precious metal-free electrocatalysts in the promotion of electrochemical water oxidation is essential for the sustainable use of renewable energy. Herein, an integrated, S-doped MnO x /Mn film developed on carbon paper (CP) formed by a two-step transformation approach that includes template-free electrodeposition and in-situ electrochemical oxidation is employed as an efficient oxygen evolution reaction (OER) electrocatalyst. The doping of S and in-situ electro-oxidation lead to a tailored electronic structure and phase composition , which endow the composite electrode with a significantly enhanced OER catalytic performance. This S-doped integrated electrode perfectly combines highly active MnO x outer layers with conductive metallic Mn inner layers to offer abundant catalytic interfaces and electronic paths, leading to favorable reaction kinetics. As a result, the optimal S-doped MnO x /Mn/CP offers a low overpotential of 435 mV at 10 mA cm −2 with a Tafel slope of 89.97 mV dec −1 as well as improved stability. Impressively, a highly intrinsic catalytic activity with a turnover frequency of 0.0112 s −1 is obtained for S-doped MnO x /Mn/CP, which is 4.2-fold higher than that of MnO x /Mn/CP. S doping plays a critical role in stabilizing the Mn III O x active phase and is ultimately responsible for the enhanced catalytic performance. This work provides an integrated design concept and S doping approach suitable for boosting the OER catalytic performance of MnO x .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Hairus Abdullah,Riski Titian Ginting,Refi Ikhtiari,Noto Susanto Gultom,Hardy Shuwanto,Dong-Hau Kuo
Configurational entropy composites of In-doped Zn(O,S)/Zn-doped In(OH) 3-x S x has been synthesized with a one-step hydrothermal method and carefully characterized with XRD , XPS , SEM, TEM, DRS , PL , EIS , TPC , CV , and MS analyses. The composites were prepared with different sulfur amounts to obtain the optimum performance of visible-light photocatalytic HER . The primary phases of ZnS and In(OH) 3 were formed after the hydrothermal process. However, the results indicated In and O were doped into ZnS lattice and induced lower bandgap values (~2.71–2.84 eV) which are active in visible-light illumination. Simultaneously, the excess Zn and S were also doped to In(OH) 3 with lower bandgap values (~3.38–4.63 eV). The variation of bandgap values is due to the hybridization of In 5s5p to Zn 4s4p and O 2p to S 3p orbitals. As a result, In-doped Zn(O,S) and Zn-doped In(OH) 3-x S x will be a visible-light active material for photoreaction and a favorable phase for electron transfer , respectively. Furthermore, it is also related to a possible antisite-defect formation with I n Z n + to help the electron trapping and enhance the photocarrier separation, leading to an efficient photocatalytic activity . ZI-S1 with additional 5-mmol thioacetamide was found as the catalyst with the highest HER performance which achieved 730 μmol/g·h under visible-light illumination. A plausible photocatalytic HER mechanism is discussed and proposed in this work.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 42
·22065-22074
·
IF 11.301
Hongling Guo,Gang Wang,Rutao Meng,Yali Sun,Siyu Wang,Shengli Zhang,Jianyu Wu,Li Wu,Guangxing Liang,Hui Li,Yi Zhang
A Li+-doping strategy is a promising route for achieving highly efficient Cu2ZnSn(S,Se)4 (CZTSSe) photovoltaic devices with a large grain absorber layer, high p-type carrier concentration and good band alignment at the Cu2ZnSn(S,Se)4/CdS interface. However, Li+-doped CZTSSe solar cells based on in situ and pre-deposition doping strategies reported thus far generally suffer from massive lithium losses and sodium rejection due to the soda-lime glass substrate. Therefore, simultaneously fulfilling the goals of simple and efficient Li+-doping remains a major technical challenge, which may be addressed, as we demonstrate here, with the development of a Se&LiF co-selenization process. By engineering the band alignment of the Cu2ZnSn(S,Se)4/CdS interface through the Se&LiF co-selenization process, an encouraging efficiency of 11.63% with an open-circuit voltage deficit of 0.583 V has been reached. Furthermore, the crystallinity of the absorber layer and the distribution of copper are improved, and a more copper-poor CZTSSe surface is formed. This novel Li+-doping strategy introduces a new approach towards the goal of high-performance CZTSSe solar cells compatible with a simple manufacturing process and excellent performance.
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JOURNAL OF BIOTECHNOLOGY
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2020
·
IF 3.503
Chun-Yue Weng,Dan-Na Wang,Shan-Yun Ban,Qiu-Yao Zhai,Xin-Yi Hu,Feng Cheng,Ya-Jun Wang,Yu-Guo Zheng
( S )-2-chlorophenylglycine methyl ester (( S )- 1 ) is a key chiral building block of clopidogrel, which is a widely administered antiaggregatory and antithrombotic drug. Herein, Protease 6SD was covalently immobilized on multi-walled carbon nanotubes (MWCNT), and the as-prepared immobilizate P-6SD@NH 2 -MWCNT was applied in the enantioselective resolution of ( R,S )- 1 to yield ( S )- 1 . In order to overcome the poor solubility of ( R,S )- 1 in aqueous solution, a novel triphasic reaction system constituting P-6SD@NH 2 -MWCNT, aqueous phase and methyl tert -butyl ether (MTBE) as the organic phase was constructed, which simultaneously improved the substrate solubility and the immobilizate recyclability. Under the optimized reaction conditions, P-6SD@NH 2 -MWCNT catalyzed 10 mM ( R,S )- 1 for 2 h, yielding optically pure ( S )- 1 (>99.0 % ee s ) with 70.74 % conversion of the ( R,S )- 1 . Moreover, P-6SD@NH 2 -MWCNT can be reused for 15 batches, displaying an exquisite recycling performance. It is for the first time that enantiomerically pure ( S )- 1 was successfully synthesized by protease-catalyzed one-step resolution.
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PubMed
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Zhong-Qiu Liu,Sheng-Nan Li,Qing-Shuai Zeng,Yu-Jing Liu,Jin-Mao You,An-Guo Ying
The preparation of mesoporous poly(ionic liquid)s (MPILs) is critically fundamental for the design of heterogeneous catalysts, whereas traditional methods are difficult to obtain these materials with both well-defined mesoporous structure and unique functionality. Here, HClO 4 -functionalized MPILs with well-defined mesoporous structure were successfully fabricated, in which the alkene-modified Fe 3 O 4 nanoparticles as structural reinforcer play a vital role for mesoporous structure formation. The MPILs were characterized by N 2 adsorption/desorption, scanning electron microscope (SEM), transmission Electron Microscope (TEM), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and vibration sample magnetometry (VSM), and the results confirm that MPILs possess moderate surface area, well-defined mesoporosity, abundant active ionic centers, as well as efficient magnetic recovery. The resulting MPILs show excellent catalytic activity for condensation reaction and Knoevenagel condensation. The kinetic study reveals that the excellent catalytic activity of MPILs is attributed to the synergistic catalysis of mesoporous confinement effect and hydrogen proton from MPILs, albeit with mass transfer resistance produced by mesoporous channels. Further, the catalyst can be recovered using an external magnetic field and reused at least 10 times without a considerable decrease in its catalytic activity. Finally, alkene-modified Fe 3 O 4 nanoparticle-mediated mesoporous construction promotes a textural engineering approach to the development of novel mesoporous materials for other applications.
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Materials Today Energy
·
2020
·
IF 5.604
C. Xu,J. Zhan,Z. Wang,X. Fang,J. Chen,F. Liang,H. Zhao,Y. Lei
Na–CO 2 batteries are prospective in energy storage and CO 2 recycling applications; development of a high-efficiency, low-cost electrocatalyst to promote CO 2 reduction and carbonate decomposition is extremely vital for practical Na–CO 2 batteries. Herein, a highly efficient cathode catalyst for rechargeable hybrid Na–CO 2 batteries is successfully synthesized by encapsulating highly dispersed Co/Co 9 S 8 nanoparticles into carbon skeletons, consisting of biomass-derived S, N-co-doped hierarchically porous carbon (Co/Co 9 S 8 @SNHC). The conductive and hierarchically porous framework structure of the Co/Co 9 S 8 @SNHC can not only accelerate electron transport , electrolyte infiltration , and CO 2 diffusion but also can inhibit overgrowth and agglomeration of Co/Co 9 S 8 nanoparticles and expose numerous high density of active sites, as well as offer sufficient space to store discharge products. Benefiting from the synergistic effect among S and N dopants , carbon defects, and Co/Co 9 S 8 nanoparticles in robust porous carbon structure, the hybrid Na–CO 2 batteries displayed a low charge overpotential (only ~0.32 V) at 0.2 mA/cm 2 and repeatedly charged and discharged over 200 cycles at 0.1 mA/cm 2 . Besides, an ultrahigh areal capacity of ~18.9 mAh/cm 2 was obtained at 0.5 mA/cm 2 , the highest value to date for Na–CO 2 batteries. Meanwhile, the hybrid Na–CO 2 battery charging from Na 2 CO 3 @C catalytic cathode demonstrated the high catalytic activity of biomass-derived S,N-co-doped hierarchically porous carbon (Co/Co 9 S 8 @SNHC) for CO 2 reduction and carbonate decomposition. Given this finding, this work might open up a potential avenue for the reasonable design of low-cost and highly efficient catalysts for advanced metal-CO 2 batteries systems.
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NAUNYN-SCHMIEDEBERGS ARCHIVES OF PHARMACOLOGY
·
2019
·Vol. 393
·期 6
·967-978
·
IF 2.058
Rong Rong,Zhang Rui-zhen,Wang Xin,Dan Yu-han,Zhao Yun-li,Yu Zhi-guo
R -/ S -2-(2-hydroxypropanamido) benzoic acid ( R -/ S -HPABA), marine-derived anti-inflammatory antiplatelet drugs, were initially synthesised in our group. However, preliminary research showed that R -/ S -HPABA were eliminated rapidly because of extensive hydroxylation metabolism of phenyl ring in vivo. In order to reduce significant hydroxylation metabolism to improve pharmacological activity and bioavailability, trifluoromethyl group was incorporated into R -/ S -HPABA to synthesise R -/ S -2-(2-hydroxypropanamido)-5-trifluoromethyl benzoic acid ( R -/ S -HFBA), respectively. The purposes of this study were to report the synthesis of R -/ S -HFBA and compare the anti-inflammatory antiplatelet effect and pharmacokinetic properties of R -/ S -HFBA with those of R -/ S -HPABA. Carrageenan-induced rat paw edema assay was used for the evaluation of the anti-inflammatory activity. R -/ S -HFBA showed better results in inhibiting edema and were able to prolong the anti-inflammatory effect after carrageenan injection. The antiplatelet aggregation activity of R -/ S -HFBA and R -/ S -HPABA was studied on arachidonic acid-induced platelet aggregation of rabbit platelet-rich plasma. The aggregation inhibition rate of R- / S -HFBA was significantly ( p < 0.05) higher than that of R- / S -HPABA, respectively. Molecular docking study revealed that R -/ S -HFBA possess more potent binding affinity with COX-1/COX-2 than R -/ S -HPABA, respectively, and that the presence of trifluoromethyl group leads to increase in activity of R -/ S -HFBA. R -/ S -HFBA also afford more favorable pharmacokinetic properties than R- / S -HPABA, respectively, such as higher C max , larger AUC 0-∞ , and longer t 1/2 , which, as expected, are more metabolically stable.
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高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Shizong Wang,Haiyang Liu,Jianlong Wang
In this study, nitrogen, sulfur and oxygen co-doped carbon armored cobalt sulfide (Co/Co 9 S 8 @N-S-O-C) composite was synthesized, characterized and used to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). SMX (0.04 mM) can be completely degraded within 20 min in the presence of 0.8 mM PMS and 0.1 g/L Co/Co 9 S 8 @N-S-O-C composite. The first-order kinetics constant of SMX degradation was 0.307 min -1 , and the mineralization of SMX was 30.1 %. The Quenching experiments of the free radicals and the identification of degradation products demonstrated that sulfate radicals played a dominant role in SMX degradation. The degradation rate of SMX increased with temperature, and activation energy was calculated to be 48.6 kJ/mol. The degradation rate of SMX increased firstly then decreased with increase of pH. Chloridion and humic acid decreased the degradation rate of SMX no matter what their initial concentration was. The effect of carbonate on SMX degradation depended on its initial concentration. Co/Co 9 S 8 @N-S-O-C composite showed good stability, the removal efficiency of SMX was 98.4 % in the fifth experiment. Based on the characterization results of the catalyst before and after use, it was concluded that cobalt, sulfur, pyridnic N and graphitic N were responsible for PMS activation.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2019
·
IF 3.206
Kwabena Agyarko Sarpong,Kun Zhang,Yu Luan,Yunfei Cao,Wanzhen Xu
Tetrabromobisphenol-S (TBBPS) is a Brominated Flame Retardants (BFRs). TBBPS in trace quantities is lethal and do not only alter the normal performance of the endocrine system but can directly or indirectly provoke hepatoxicity and carcinogenic diseases. Herein, we fabricate a facile electrochemical sensor and investigate its application towards the determination of TBBPS through imprinting technique. TBBPS imprinting was carried out in the presence of methacrylic acid (MAA) and 4-aminothiophenol (4-ATP) functional monomers (DiM) over gold nanoparticles (AuNPs) modified carbon paste electrode (CPE). Transmission electron microscopy (TEM) was used to characterize the imprinted sensor. Performance was thoroughly investigated using both cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The proposed sensor showed detection behavior towards TBBPS in standard solutions with different concentrations range of 0.1 nM-10 nM and with a detection limit of 0.029 nM. The developed MIP(DiM)@AuNPs/CPE sensor had enhanced recognition capacity compared to MIP electrochemical sensors developed with a mono functional monomer (MIP(MoM)@AuNPs/CPE) and non-imprinted sensors. In addition, the low cost; easier preparation; excellent stability; and good selectivity of MIP(DiM)@AuNPs/CPE electrochemical sensor makes it an attractive alternative to high instrumentation detection techniques.
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Materials Express
·
2023
·Vol. 13
·期 11
·1922-1928
·
IF 0.7
Yang Jing,Deng Qiuhui,Luo Chunhua,Yang Aofeng,Luo Xiaohu,Guo Meng,Fu Lichun,Zhen Deshuai,Zhou Huang
Holmium (Ho) modified TiO2 (Ho–TiO2) nanocomposites have been prepared by a sol–gel process, and were used as an effective adsorbent and matrix for the enrichment and analysis of bisphenol S and Indigo by matrix-assisted laser desorption/ionization
time-of-flight mass spectrometry (MALDI-TOF MS). The low detection limits of bisphenol S (BPS) and Indigo (ID) are 0.1 pg·mL−1 and 5 pg·mL−1, respectively. Extremely BPS detection could be achieved in tea samples with good recovery (81.5–93.0%).
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