Orbital-regulated interfacial electronic coupling endows Ni3N with superior catalytic surface for hy

• 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 Q
• 机 构: Hefei National Laboratory for Physical Science at the Microscale,Department of Chemistry,University
• 出 处: 中国科学:化学（英文版）
• 发表日期: 2020年11期
• 关键词: hydrogen evolution reaction orbital regulation interfacial electronic coupling N

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 catalysis.Herein,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 dopants.The prepared O-Ni3N catalyst delivers an overpotential of 55 mV at 10 mA cm-2,very close to the commercial Pt/C.Refined structural characterization indicates the oxygen incorporation can decrease the electron densities around the Ni sites.Moreover,density functional theory calculation further proves the oxygen incorporation can create more unoccupied orbitals with lower energy and superior orientation for water adsorption and dissociation.The concept of orbital-regulated interfacial electronic coupling could offer a unique approach for the rational design of hydrogen evolution catalysts and beyond.