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interfacial electronic interaction enabling exposed Pt(110)facets with high specific activity in hydrogen evolution reaction

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Nano Research 2023年第1期16卷 174-180页

作者： Sicong Qiao Qun He Quan Zhou Yuzhu Zhou Wenjie Xu Hongwei Shou Yuyang Cao Shuangming Chen Xiaojun Wu Li Song National Synchrotron Radiation Laboratory CAS Center for Excellence in NanoscienceUniversity of Science and Technology of ChinaHefei 230026China Hefei National Laboratory for Physical Science at the Microscale Collaborative Innovation of Center of Chemistry for Energy Materials(iChEM)School of Chemistry and Materials SciencesUniversity of Science and Technology of ChinaHefei 230026China

To achieve a complete industrial chain of hydrogen energy,the development of efficient electrocatalysts for hydrogen evolution reaction(HER)is of great concerns.Herein,a nickel nitride supported platinum(Pt)catalyst with highly exposed Pt(110)facets(Pt_((110))-Ni_(3)N)is obtained for catalyzing HER.Combined X-ray spectra and density functional theory studies demonstrate that the interfacial electronic interaction between Pt and Ni3N support can promote the hydrogen evolution on Pt(110)facets by weakening hydrogen adsorption.As a result,the Pt_((110))-Ni_(3)N catalyst delivers an obviously higher specific activity than commercial 20 wt.%Pt/C in acidic media.This work suggests that the suitable interface modulation may play a vital role in rationally designing advanced electrocatalysts.

关键词： interfacial electronic interaction hydrogen evolution reaction X-ray spectroscopy Pt(110)facets density functional theory

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The discovery of interfacial electronic interaction within cobalt boride@MXene for high performance lithium-sulfur batteries

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Chinese Chemical Letters 2021年第7期32卷 2249-2253页

作者： Bin Guan Xun Sun Yu Zhang Xian Wu Yue Qiu Maoxu Wang Lishuang Fan Naiqing Zhang State Key Laboratory of Urban Water Resource and Environment School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China Academy of Fundamental and Interdisciplinary Sciences Harbin Institute of TechnologyHarbin 150001China

Lithium-sulfur battery is strongly considered as the most promising next-generation energy storage system because of the high theoretical specific capacity.The serious"shuttle effect"and sluggish reaction kinetic limited the commercial application of lithium-sulfur battery.Many hetero structure s were applied to accelerate polysulfides conversion and suppress their migration in lithium-sulfur batteries.Nevertheless,the effect of the interface in heterostructure was not clear.Here,the Co_(2)B@MXene heterostructure is synthesized through chemical reactions at room temperature and employed as the interlayer material for Li-S batteries.The theoretical calculations and experimental results indicate that the interfacial electronic interaction of Co_(2)B@MXene induce the transfer of electrons from Co_(2)B to MXene,enhancing the catalytic ability and favoring fast redox kinetics of the polysulfides,and the theoretical calculations also reveal the underlying mechanisms for the electron transfer is that the two materials have different Fermi energy levels.The cell with Co_(2)B@MXene exhibits a high initial capacity of1577 mAh/g at 0.1 C and an ultralow capacity decay of 0.0088%per cycle over 2000 cycles at 2 C.Even at5.1 mg/cm^(2) of sulfur loading,the cell with Co_(2)B@MXene delivers 5.2 mAh/cm^(2) at 0.2 C.

关键词： Co_(2)B@MXene Separator interfacial electronic interaction Catalytic activity Lithium-sulfur batteries

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Synergistic effects of CeO_(2)/Cu_(2)O on CO catalytic oxidation:electronic interaction and oxygen defect

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Journal of Rare Earths 2022年第8期40卷 1211-1218页

作者： Chengyan Ge Jingfang Sun Qing Tong Weixin Zou Lulu Li Lin Dong School of Chemistry and Chemical Engineering Yancheng Institute of TechnologyYancheng 224051China Jiangsu Key Laboratory of Vehicle Emissions Control Center of Modern AnalysisSchool of the EnvironmentNanjing UniversityNanjing 210093China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

For CO catalytic oxidation,Cu and Ce species are of great importance,between which the synergistic effect is worth investigating.In this work,CeO_(2)/Cu_(2)O with Cu_(2)O {111} and {100} planes were comparatively explored on CO catalytic oxidation to reveal the effects of interfacial electronic interactions and oxygen defects.The activity result demonstrates that CeO_(2)/o-Cu_(2)O {111} has superior performance compared with CeO_(2)/c-Cu_(2)O {100}.Credit to the coordination unsaturated copper atoms(Cu_(CUS)) on oCu_(2)O {111} surface,the interfacial electronic interactions on CeO_(2)/o-Cu_(2)O {111} are more obvious than those on CeO_(2)/c-Cu_(2)O {100},leading to richer oxygen defect generation,better redox and activation abilities of CO and O_(2) reactants.Furthermore,the reaction mechanism of CeO_(2)/o-Cu_(2)O {111} on CO oxidation is revealed,i.e.,CO and O_(2) are adsorbed on the Cucus on Cu_(2)O {111} and oxygen defect of CeO_(2),respectively,and then synergistically promote the CO oxidation to CO_(2).The work sheds light on the designing optimized ceria and copper-based catalysts and the mechanism of CO oxidation.

关键词： CeO_(2)/Cu_(2)O{111}{100} Synergistic effect interfacial electronic interaction Oxygen defect CO oxidation Rare earths

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单原子催化剂促进Li-CO_(2)电池中Li_(2)CO_(3)/C的快速分解

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Science China Materials 2021年第9期64卷 2139-2147页

作者：周丽姣王辉张坤齐亚琴沈超金婷谢科予 School of Materials Science and Engineering Northwestern Polytechnical UniversityXi’an 710072China

锂-二氧化碳(Li-CO_(2))电池充分利用温室气体CO_(2),其理论能量密度高达1876 W h kg^(-1),使之被认为是未来储能系统的潜在候选者和锂离子电池的替代品.然而,放电产物(Li_(2)CO_(3)/C)的聚集以及缓慢的反应动力学特征,导致其极化高、... 详细信息

锂-二氧化碳(Li-CO_(2))电池充分利用温室气体CO_(2),其理论能量密度高达1876 W h kg^(-1),使之被认为是未来储能系统的潜在候选者和锂离子电池的替代品.然而,放电产物(Li_(2)CO_(3)/C)的聚集以及缓慢的反应动力学特征,导致其极化高、循环寿命短.因此,研究与开发高效催化剂来促进Li_(2)CO_(3)/C分解尤为重要.其中,单原子催化剂(SACs)中金属原子利用率高、界面电子相互作用强,因而被视为有前途的多相催化剂.本文设计合成了均匀锚定在氮掺杂还原氧化石墨烯上的单金属原子催化剂(Fe_(1)/N-rGO,Co1/N-rGO和Ni_(1)/N-rGO),并深入研究了它们对Li_(2)CO_(3)/C分解的催化分解活性.其中,Fe_(1)/N-rGO在100 mA g^(-1)时放电比容量高达16,835 mA h g^(-1),且在400 mA g^(-1)时以2.30 V的放电电压稳定循环170次,明显优于其他催化剂.这项工作揭示了SACs在Li-CO_(2)电池中取得的进步,并为实现高性能Li-CO_(2)电池提供了有效的方法.

关键词： Li-CO_(2)batteries single-atom catalysts Li_(2)CO_(3)/C interfacial electronic interaction M-N-C bonds

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