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Orbital-regulated interfacial electronic coupling endows Ni3N with superior catalytic surface for hydrogen evolution reaction

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Science China Chemistry 2020年第11期63卷 1563-1569页

作者： Yanyan Fang Da Sun Shuwen Niu Jinyan Cai Yipeng Zang Yishang Wu Linqin Zhu Yufang Xie Yun Liu Zixuan Zhu Amirabbas Mosallanezhad Di Niu Zheng Lu Junjie Shi Xiaojing Liu Dewei Rao Gongming Wang Yitai Qian Hefei National Laboratory for Physical Science at the Microscale Department of ChemistryUniversity of Science&Technology of ChinaHefei 230026China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China

The interstitial structure and weak Ni-N interaction of Ni3N lead to high unoccupied d orbital energy and unsuitable orbital orientation,which consequently results in weak orbital coupling with H2O and slow water dissociation kinetics for alkaline hydrogen evolution ***,we successfully lower the unoccupied d orbital energy of Ni3N to strengthen the interfacial electronic coupling by employing the strong electron pulling capability of oxygen *** prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm−2,very close to the commercial Pt/*** structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni ***,density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and *** concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.

关键词： hydrogen evolution reaction orbital regulation interfacial electronic coupling Ni3N electrocatalysts

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Optimizing interfacial electronic coupling with metal oxide to activate inert polyaniline for superior electrocatalytic hydrogen generation

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Carbon Energy 2019年第1期1卷 77-84页

作者： Zhen-Feng Huang Jiajia Song Yonghua Du Shuo Dou Libo Sun Wei Chen Kaidi Yuan Zhengfei Dai Xin Wang School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingaporeSingapore Singapore-HUJ Alliance for Research and Enterprise NEW-CREATE Phase IICampus for Research Excellence and Technological Enterprise(CREATE)SingaporeSingapore Institute of Chemical and Engineering Sciences A*STARJurong IslandSingapore Department of Chemistry National University of SingaporeSingaporeSingapore School of Materials Science and Engineering Nanyang Technological UniversitySingaporeSingapore

Tuning and optimization of electronic structures and related reaction energetics are critical toward the rational design of efficient ***,experimental and theoretical calculation demonstrate the originally inert N site within polyaniline(PANI)can be activated for hydrogen evolution by proper d-πinterfacial electronic coupling with metal *** a result,the assynthesized WO3 assemblies@PANI via a facile redox-induced assembly and in situ polymerization,exhibits the electrocatalytic production of hydrogen better than other control samples including W18O49@PANI and most of the reported nobel-metal-free electrocatalysts,with low overpotential of 74 mV at 10 mA·cm−2 and small Tafel slope of 46 mV·dec−1 in 0.5M H2SO4(comparable to commercial Pt/C).The general efficacy of this methodology is also validated by extension to other metal oxides such as MoO3 with similar improvements.

关键词： hydrogen evolution interfacial electronic coupling metal oxide N-H bond polyaniline

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