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In-situ reconstruction of catalysts in cathodic electrocatalysis: New insights into active-site structures and working mechanisms

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Journal of Energy Chemistry 2022年第7期31卷 414-436,I0011页

作者： Wenbiao Zhang Yang Yang Yi Tang Qingsheng Gao College of Chemistry and Materials Science and Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632GuangdongChina Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsLaboratory of Advanced Materials and Collaborative Innovation Center of Chemistry for Energy Materials(iCHEM)Fudan UniversityShanghai 200433China

Cathodic electrocatalytic reactions, such as hydrogen evolution and CO_(2)/N_(2) reduction, are the key processes that store intermittent electricity into stable chemical energy. Although a great progress has been made to boost activity and selectivity via elaborative catalyst design, the structure–property relationships have not been sufficiently understood in the context of surface reconfiguration under working conditions. Recent efforts devoted to tracking dynamic evolution of electrocatalysts using in-situ and/or operando techniques gave new insights into the real structure and working mechanism of active sites,and provided principles to design better catalysts. The achievement of cathodic electrocatalysts in this subject is herein summarized, focusing on the correlations between reconstructed surface and electrocatalytic performance. Briefly, the thermodynamics of reconstruction at cathodes is discussed at first, and then the representative progresses in H_(2) evolution and CO_(2)/N_(2) reduction are introduced in sequence to acquire insights into electrochemical processes on in-situ reconfigured surfaces or interfaces. Finally, a perspective is offered to guide future investigations. This review is anticipated to shed some new light on in-depth understanding cathodic electrocatalysis and exploiting prominent electrocatalysts.

关键词： Hydrogen evolution reaction CO_(2)reduction reaction Nitrogen reduction reaction In-situ reconstruction Electronic configurations valence states Topological changes

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Enhancing the dynamic electron transfer of Au species on wormhole-like TS-1 for boosting propene epoxidation performance with H_(2) and O_(2)

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Green Energy & Environment 2020年第4期5卷 433-443页

作者： Dong Lin Xiuhui Zheng Xiang Feng Nan Sheng Zhaoning Song Yibin Liu Xiaobo Chen Zhenping Cai De Chen Chaohe Yang State Key Laboratory of Heavy Oil Processing China University of PetroleumQingdao266580China Department of Chemical Engineering Norwegian University of Science and TechnologyTrondheim7491Norway

Engineering unique electronic structure of catalyst to boost catalytic performance is of prime scientific and industrial importance.Herein,the identification of intrinsic electronic sensitivity for direct propene epoxidation was first achieved over highly stable Au/wormhole-like TS-1 catalyst.Results show that the electron transfer of Au species can be regulated by manipulating the dynamic evolutions and contents of Au valence states,thus resulting in different catalytic performance in 100 h time-on-stream.By DFT calculations,kinetic analysis and multicharacterizations,it is found that the Au^(0) species with higher electronic population can easily transfer more electrons to activate surface O_(2) compared with Au^(1+) and Au^(3+) species.Moreover,there is a positive correlation between Au^(0) content and activity.Based on this correlation,a facile strategy is further proposed to boost Au^(0) percentage,resulting in the reported highest PO formation rate without adding promoters.This work harbors tremendous guiding significance to the design of highly efficient Au/Ti-containing catalyst for propene epoxidation with H_(2) and O_(2).

关键词： Electron transfer valence states Evolution Propene epoxidation DFT

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COLOUR-CHANGING MECHANISM IN P_2O_5-Nb_2O_5-Li_2O NONCRYSTALLINE SYSTEM

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Journal of Wuhan University of Technology(Materials Science) 1989年第2期4卷 15-23页

作者：崔万秋阮立坚陈丹平 Wuhan University of Technology

Raman, IR spectra, RDF and visible spectrum were used to study the glass structure and the valence states of niobium ions in P_2O_5-Nb_2O_5-Li_2O noncrystalling system. The colour-changing mechanism was studied. For 10Nb_2O_5xP_2O_5(90-x)Li_2O (x=40,45,50,55) system glasses, it was known that the glass colout changing from light gold-yellow to blue with increasing is aroused by the Nb^(3+) ion increasing, not by the change of niobium ion coordination.

关键词： Glass structure valence states Colour,Coordination

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DFT Study of the Effects of Valance states of Mo and Surface Hydroxyl of MoOx/Al2O3 Catalysts on Ethylene Polymerization

DFT Study of the Effects of Valance States of Mo and Surface...

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13th Asian Chemical Congress

作者： CAO Xiaochun CHENG Ruihua DONG Qi HE Xuelian LIU Boping~* State Key Lab of Chemical Engineering EUST Meilong Road 130 ShangHai 200237 China

＜正＞Supported MoOx catalyst with low toxicity has potential to replace highly toxic Phillips（CrOx/SiO2） catalyst.Ethylene polymerization on MoOx/Al2O3 catalyst was investigated using density function theory（DFT）... 详细信息

关键词： MoOx catalyst DFT valence states Surface hydroxyl

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