Accelerating water dissociation kinetics of Ni3N by tuning interfacial orbital coupling

作     者：Yishang Wu Yufang Xie Shuwen Niu Yipeng Zang Jinyan Cai Zenan Bian Xuanwei Yin Yanyan Fang Da Sun Di Niu Zheng Lu Amirabbas Mosallanezhad Huijuan Wang Dewei Rao Hongge Pan Gongming Wang Yishang Wu;Yufang Xie;Shuwen Niu;Yipeng Zang;Jinyan Cai;Zenan Bian;Xuanwei Yin;Yanyan Fang;Da Sun;Di Niu;Zheng Lu;Amirabbas Mosallanezhad;Huijuan Wang;Dewei Rao;Hongge Pan;Gongming Wang

作者机构：Hefei National Laboratory for Physical Science at the MicroscaleDepartment of ChemistryUniversity of Science and Technology of ChinaHefei 230026China Experimental Center of Engineering and Material ScienceUniversity of Science and Technology of ChinaHefei 230026China School of Materials Science and EngineeringJiangsu UniversityZhenjiang 212013China Institute of Science and Technology for New EnergyXi’an Technological UniversityXi’an 710021China School of Materials Science and EngineeringState Key Laboratory of Silicon MaterialsZhejiang UniversityHangzhou 310027China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2021年第14卷第10期

页      面：3458-3465页

核心收录：

学科分类：0808[工学-电气工程] 081704[工学-应用化学] 0809[工学-电子科学与技术（可授工学、理学学位）] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：The work was supported by the National Natural Science Foundation of China(Nos.21771169 and 11722543) the National Key Research and Development Program of China(No.2017YFA0206703) Anhui Provincial Natural Science Foundation(No.BJ2060190077) Collaborative Innovation Program of Hefei Science Center,CAS,and the Fundamental Research Funds for the Central Universities(Nos.WK2060190074,WK2060190081,WK2310000066,and WK2060000015) 

主　　题：unoccupied d orbitals Ni_(3)N Cr-N_(6)doping interfacial orbital coupling hydrogen evolution reaction 

摘      要：The high unoccupied d band energy of Ni_(3)N basically results in weak orbital coupling with water molecule,consequently leading to slow water dissociation ***,we demonstrate Cr doping can downshift the unoccupied d orbitals and strengthen the interfacial orbital coupling to boost the water dissociation *** prepared Cr-Ni_(3)N/Ni displays an impressive overpotential of 37 mV at 10 mA·cmgeo-2,close to the benchmark Pt/C in 1.0 M KOH *** structural analysis reveals the Cr dopant exists as the Cr-N_(6)states and the average d band energy of Ni_(3)N is also *** functional theory calculation further confirms the downshifted d band energy can strengthen the orbital coupling between the unpaired electrons in O 2p and the unoccupied state of Ni 3d,which thus facilitates the water adsorption and *** work provides a new concept to achieve on-demand functions for hydrogen evolution catalysis and beyond,by regulating the interfacial orbital coupling.