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Unraveling the stabilization mechanism of solid electrolyte interface on ZnSe by rGO in sodium ion battery

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Journal of Energy Chemistry 2021年第3期30卷 124-130页

作者： Shuang Men Hui Zheng Dejun Ma Xiaolian Huang xiongwu kang School of Environment and Energy South China University of TechnologyGuangzhou 510006GuangdongChina Department of Chemical Engineering Northwest UniversityXi'an 710069ShaanxiChina School ofPhamacy Guangdong Pharmaceutical UniversityGuangzhou 510006GuangdongChina College of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006GuangdongChina

Transition metal selenides have been widely studied as anode materials of sodium ion batteries(SIBs),however,the investigation of solid-electrolyte-interface(SEI)on these materials,which is critical to the electrochemical performance of SIBs,remains at its *** in this paper,ZnSe@C nanoparticles were prepared from ZIF-8 and the SEI layers on these electrodes with and without reduced graphene oxide(rGO)layers were examined in details by X-ray photoelectron spectroscopies at varied charged/discharged *** is observed that fast and complicated electrolyte decomposition reactions on ZnSe@C leads to quite thick SEI film and intercalation of solvated sodium ions through such thick SEI film results in slow ion diffusion kinetics and unstable electrode ***,the presence of rGO could efficiently suppress the decomposition of electrolyte,thus thin and stable SEI film was ***@C electrodes wrapped by rGO demonstrates enhanced interfacial charge transfer kinetics and high electrochemical performance,a capacity retention of 96.4%,after 1000 cycles at 5 A/*** study might offer a simple avenue for the designing high performance anode materials through manipulation of SEI film.

关键词： ZIF-8 Zinc selenide Transition metal selenide Reduced graphene oxide XPS Solid electrolyte interface Sodium ion batteries

Pt-Co single atom alloy catalysts: Accelerated water dissociation and hydrogen evolution by strain regulation

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Journal of Energy Chemistry 2022年第6期31卷 44-53,I0002页

作者： Rendian Wan Mi Luo Jingbo Wen Shilong Liu xiongwu kang Yong Tian School of Pharmacy Guangdong Pharmaceutical UniversityGuangzhou 510006GuangdongChina New Energy Research Institute School of Environment and EnergySouth China University of TechnologyHigher Education Mega CenterGuangzhou 510006GuangdongChina

The alkaline hydrogen evolution reaction(HER) on Pt-based catalysts is largely limited by the slow water dissociation kinetics. Pt-based single atom alloy catalysts(SAAC) with water dissociation sites have been demonstrated as excellent alkaline HER catalysts. However, the regulation of their activity and stability at the atomic scale is still a great challenge. Herein, the kinetic and stability issues are successfully resolved via engineering the electronic structure of Pt-Co SAAC by Au-induced tensile strain. The atomic dispersion of Co into the Pt shell was confirmed by extended X-ray absorption fine structure and the electronic structure and catalytic HER performance was modulated by the tensile strain induced by the Pt shell thickness. An inverse volcano-type relation between HER activity and surface strain was *** functional theory(DFT) calculations reveal that the Au-induced tensile strain on Pt-Co shell can not only boost the adsorption and dissociation kinetics of water at Co site by upshifting the dband and promoting the electron transfer, but also downshift the d-band center of Pt in Pt-Co shell, leading to optimized H* adsorption/desorption. The champion catalyst provides an overpotential of only 14 m V at the current density of 10 mA cm^(-2). This work not only provides an effective strategy for the construction of single-atom alloy electrocatalysts for high performance toward alkaline HER but also sheds light on the understanding of the reaction mechanism at the atomic level.

关键词： Hydrogen evolution reaction Single atom alloy Strain DFT calculation d-band

Modulating surface oxygen species via facet engineering for efficient conversion of nitrate to ammonia

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Journal of Energy Chemistry 2023年第3期78卷 211-221,I0007页

作者： Wenye Zhong Zhiheng Gong Zuyun He Nian Zhang xiongwu kang Xianwen Mao Yan Chen School of Environment and Energy State Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhou 510006GuangdongChina State Key Laboratory of Functional Materials for Informatics Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China Department of Materials Science and Engineering National University of SingaporeSingapore 119077Singapore Institute of Functional Intelligent Materials National University of SingaporeSingapore 119077Singapore Centre for Advanced 2D Materials National University of SingaporeSingapore 119077Singapore

Electrochemical reduction of nitrate,a common pollutant in aquatic environment,to valuable ammonia(NO3-RR) using renewably-sourced electricity has attracted widespread interests,with past efforts mainly focused on designing electrocatalysts with high activity and *** detailed correlation between catalyst properties and NO3-RR kinetics,nevertheless,is still not fully *** this work,we modulate the surface oxygen species of Cu_(2)O via facet engineering,and systematically study the impact of these oxygen species on the NO_(3)^(-)RR *** advanced spectroscopic techniques,densi ty fu n ctional theory calculations and molecular dynamics simulations,we find that while oxygen vacancies on Cu_(2)O(111) surface promote the adsorption of reactants and reaction intermediates,hydroxyl groups effectively inhibit the side reaction of hydrogen evolution and facilitate the hydrogenation process of *** two effects work in concert to render Cu_(2)O(111) facet the highest NO3-RR activity relative to those from other *** study provides critical insights into the synergistic effect of exposed facets and surface oxygen species on heterogeneous catalysis,and offers a generalizable,facet engineeringbased strategy for improving the performance of a variety of electrocatalysts important for renewable energy conversion.

关键词： Facet engineering Oxygen vacancy Hydroxyl group Electrochemical nitrate reduction Ammonia

Pyrrole derivatives as interlayer modifier of Li-S batteries:Modulation of electrochemical performance by molecular perturbation

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Journal of Energy Chemistry 2022年第12期75卷 164-172,I0005页

作者： Jiajv Lin Yuan Zhou Jingbo Wen Weijie Si Hongcheng Gao Gongming Wang xiongwu kang New Energy Research Institute School of Environment and EnergySouth China University of TechnologyGuangzhou 510006GuangdongChina Key Laboratory of Aqueous Environment Protection and Pollution Control of Yangtze River in Anhui of Anhui Provincial Education DepartmentCollege of Resources and EnvironmentAnqing Normal UniversityAnqing 246011AnhuiChina Hefei National Laboratory for Physical Sciences at the Microscale and Department of Chemistry University of Science&Technology of ChinaHefei 230026AnhuiChina

The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S batteries is demonstrated to be an effective strategy to overcome this ***,cobalt nanoparticles confined in nitrogen co-doped porous carbon framework(Co-CN)were developed from pyrolysis of ZIF-67 and used as interlayer of PP separator for Li-S batteries,and were functionalized by four pyrrole derivatives,1-phenylpyrrole,1-methyl pyrrole,1-(p-toluenesulfonyl)pyrrole,and 1-pyrrole,respectively,which were screened in terms of the electron-withdrawing/donating ability of the substituent groups on the pyrrolic *** impact of the molecular structure of pyrrole derivatives on the interaction with Li PSs and the electrochemical performance of Li-S batteries were explored by nuclear magnetic resonance and theoretical *** is uncovered that 1-phenylpyrrole shows the highest enhancement of redox kinetics of Li PSs,attributing to the optimal interaction with Co nanoparticles and Li ***,1-phenylpyrrole modified Co-CN interlayer enables the best electrochemical performance for the Li-S batteries,delivering a specific capacity of 562 m Ah g^(-1)at 5 C and a capacity of 538,526,and 449 m Ah g^(-1)after 500 cycles at 1,2,and 3 C,*** a high sulfur loading of 5.5 mg cm^(-2),it achieves a capacity of 440 m Ah g^(-1)after 500 cycles at 1 *** work reveals the interaction mechanism among Li PSs,Co nanoparticles and the molecular modifiers in improving the electrochemical performance of Li-S batteries.

关键词： Pyrrole derivatives Surface modification Interlayer Catalysis Redox kinetics

The electrocatalytic activity of BaTiO3 nanoparticles towards polysulfides enables high-performance lithium-sulfur batteries

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Journal of Energy Chemistry 2020年第9期29卷 208-216,I0007页

作者： Hongcheng Gao Shunlian Ning Jiasui Zou Shuang Men Yuan Zhou Xiujun Wang xiongwu kang New Energy Research Institute School of Environment and EnergySouth China University of TechnologyGuangzhou 510006GuangdongChina School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640GuangdongChina

The slow redox dynamics and dissolution of polysulfides in lithium-sulfur(Li-S)batteries result in poor rate performance and rapid decay of battery capacity,thus limiting their practical *** barium titanate(BT)nanoparticles have been reported to effectively improve the electrochemical performance of Li-S batteries due to the inherent self-polarization and high adsorption capacity of the BT nanoparticles towards *** in this paper,BT nanoparticles,behave as highly efficient electrocatalyst and demonstrate much higher redox dynamics towards the conversion reaction of polysulfides and Li2S than TiO2,as shown by both electrochemical measurements and density functional theory *** coupling of the sulfur host of the hollow and graphitic carbon flakes(HGCF)and the BT nanoparticles(HGCF/S-BT)enable excellent electrochemical performance of Li-S batteries,delivering a0.047%capacity decay per cycle in 1000 cycles at 1 C,788 mAh g^-1 at 2 C and a reversible capacity of613 mAh g^-1 after 300 cycles at a current density of 0.5 C at a S loading of 3.4 mg cm^-***/S-BT also shows great promise for practical application in flexible devices as demonstrated on the soft-packaged Li-S batteries.

关键词： Electrocatalysis Redox reaction Li-S battery Polysulfide DFT calculation

Cobalt phthalocyanine promoted copper catalysts toward enhanced electro reduction of CO_(2)to C_(2):Synergistic catalysis or tandem catalysis?

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Journal of Energy Chemistry 2024年第5期92卷 499-507页

作者： Yan Luo Jun Yang Jundi Qin kanghua Miao Dong Xiang Aidar Kuchkaev Dmitry Yakhvarov Chuansheng Hu xiongwu kang New Energy Research Institute School of Environment and EnergySouth China University of TechnologyHigher Education Mega CenterGuangzhou 510006GuangdongChina Guangdong University of Petrochemical Technology School of Chemical EngineeringMaoming 525000GuangdongChina Arbuzov Institute of Organic and Physical Chemistry FRC Kazan Scientific Center of RASArbuzov Street 8Kazan 420088Russian Federation National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina

The activity and selectivity of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to C_(2)products on metal catalysts can be regulated by molecular ***,the mechanism behind it remains elusive and ***,copper nanowires(Cu NWs)were fabricated and decorated with cobalt phthalocyanine(CoPc).The electronic interaction between the Cu NWs,CoPc,CO_(2) and CO_(2)RR intermediates were explored by density functional theory(DFT)*** was found that the selectivity and activity of CO_(2)RR towards C_(2)products on Cu NWs were considerably enhanced from 35.2%to 69.9%by surface decoration of *** calculations revealed that CO_(2)RR can proceed in the interphase between Cu substrate and CoPc,and the CO_(2)RR intermediates could synergistically bond with both Cu and Co metal centre in CuNWs-CoPc,which favours the adsorption of CO_(2),CO and CO_(2)RR intermediates,thus reducing the free energy for CO-COcoupling towards C_(2)*** synergistic interaction was further extended to phthalocyanine(Pc)and other metal phthalocyanine derivatives(MPc),where a relatively weaker synergistic interaction of COintermediates with MPc and Cu substrate and only a slight enhancement of CO_(2)RR towards C_(2) products were *** study demonstrates a synergistic catalysis pathway for CO_(2)RR,a novel perspective in interpreting the role of CoPc in enhancing the activity and selectivity of CO_(2)RR on Cu NWs,in contrast to the conventional tandem catalysis mechanism.

关键词： CO_(2)reduction reaction Raman spectroscopy Synergistic catalysis DFT calculation

Enhanced Catalytic Activity of Metal Nanomaterials by Surface and Interface Engineering

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Enhanced Catalytic Activity of Metal Nanomaterials by Surfac...

胺功能化的铜催化剂:氢键介导的电化学CO_(2)还原为C_(2)产物以及优越的可充电Zn-CO_(2)电池性能

中国化学会2019能源材料和缺陷化学研讨会

作者： xiongwu kang kanghua Miao Zhiwei Guo Fengqi Zhang Lin Huang School of Environment and Energy South China University of Technology

It is desirable to develop catalyst of high performance and low cost for the commercialization of direct formic acid/methanol fuel cells and industrial production of organic feed stocks. Here we prepared a series of PdCu nanoparticles and the size effect on the metal-support interactions are investigated in details. The interaction of PdCu alloy nanoparticles with CeO2 support induces compressive strain, down-shift of the d-band center, reduced CO binding energy and augmentation of PdO content for PdCu nanoparticles. It is concluded that the synergy of compressive strain, enhanced Pd O and oxygen vacancy remarkably promotes the catalytic performance of PdCu towards electrooxidation of formic acid, while electrooxidation of methanol on PdCu is promoted only by the oxygen vacancy. It is also noted that the surface functionalization of Ru nanoparticles by terminal and internal alkyne can equally modulate the catalytic activity towards hydrogenation of styrene by selectively covering the specific metal sites. These results demonstrate the importance of the surface and interface engineering of metal catalyst in tuning the electronic structure, surface structure and catalytic activity.

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物理化学学报 2024年第8期40卷 43-46页

作者：项东李坤振苗康华龙冉熊宇杰康雄武华南理工大学新能源研究所环境与能源学院广州510006 中国科学技术大学合肥微尺度物质科学国家研究中心化学与材料科学学院合肥230026

有机分子功能化是一种有前景的策略,用于调控电化学CO_(2)还原反应(eCO_(2)RR)的C_(2+)产物选择性和活性。然而,我们对于电化学CO_(2)还原调控机制的分子水平理解仍然不够清晰。在本文中,我们成功制备了铜纳米颗粒,并使用一系列胺类衍生... 详细信息

有机分子功能化是一种有前景的策略,用于调控电化学CO_(2)还原反应(eCO_(2)RR)的C_(2+)产物选择性和活性。然而,我们对于电化学CO_(2)还原调控机制的分子水平理解仍然不够清晰。在本文中,我们成功制备了铜纳米颗粒,并使用一系列胺类衍生物(如十六胺(HAD)、N-甲基十六胺(N-MHDA)、十六烷基二甲胺(HDDMA)和十六酰胺(PMM))对其进行功能化,以系统地研究胺表面活性剂分子结构对eCO_(2)RR选择性和活性的影响。结果表明,HDA的功能化可以将C_(2)产物和C_(2)H_(4)的法拉第效率(FE)提高至73.5%和46.4%,并且在−0.9 V ***(可逆氢电极)电位下,C_(2)产物的分电流密度为131.4 mA·cm^(−2)。理论研究发现,HDA通过与CO_(2)和eCO_(2)RR中间体之间的氢键相互作用,富集了^(*)CO_(2)、^(*)CO和其他反应中间体,降低了CO―CHO耦合反应的动力学能垒,从而促进了eCO_(2)RR向C_(2)产物的转化。当胺基的H原子被甲基取代后,氢键相互作用减弱,竞争的析氢反应加剧。PMM通过Cu―O键与Cu表面发生键合,而不是通过Cu―N键,导致Cu-PMM更倾向于产乙醇。原位拉曼光谱显示,在Cu-HDA表面,CO主要吸附在Cu的顶位吸附位点上,与在Cu表面上的桥式吸附不同,这可能是因为前者表面对CO的富集引发了CO的吸附构型变化。HDA功能化还提高了Cu催化剂的表面pH。基于Cu-HDA组装的可充电Zn-CO_(2)电池在放电电流密度为16 mA∙cm^(−2)时,最大功率密度为6.48 mW∙cm^(−2),并具有长达60 h的良好充放电稳定性。本研究的重点在于通过在分子水平上调节Cu基材料的CO_(2)RR活性和选择性,促进CO_(2)-C_(2)的转化,这可能为提高C_(2)产物的产率提供新的见解。

关键词：二氧化碳还原 CO―CHO耦合有机分子功能化原位拉曼 C_(2)产物 Zn-CO_(2)电池

维普期刊数据库博看期刊

Facile synthesis of porous germanium-iron bimetal oxide nanowires as anode materials for lithium-ion batteries

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Nano Research 2018年第7期11卷 3702-3709页

作者： xiongwu Zhong Huijuan Huan Xiaowu Liu Yan Yu Key Laboratory of Materials for Energy Conversion Chinese Academy of Sciences (CAS) Department of Materials Science and Engineering University of Science and Technology of China Hefei 230026 China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 China State Key Laboratory of Fire Science University of Science and Technology of China Hefei 230026 China

Germanium-based oxide has been found to be a promising high-capacity anode material for lithium-ion batteries （LIBs）. However, it exhibits poor electrochemical performance because of the drastic volume change during cycling. Herein, we designed porous Ge-Fe bimetal oxide nanowires （Ge-Fe-Ox-700 NWs） by a large-scale and facile solvothermal reaction. When used as the anode material for LIBs, these Ge-Fe-Ox-700 NWs exhibited superior electrochemical performance （- 1,120 mAh·g^-1 at a current density of 100 mA·g^-1） and good cycling performance （- 750 mAh·g^-1 after 50 cycles at a current density of 100 mA·g^-1）. The improved performance is due to the small NW diameter, which allows for better accommodation of the drastic volume changes and zero-dimensional nanoparticles, which shorten the diffusion length of ions and electrons.

关键词： lithium-ion batteries anode materials germanium oxide iron oxide nanowires