文献类型：期刊文献

英文题名：Efficient and Robust Hydrogen Evolution: Phosphorus Nitride Imide Nanotubes as Supports for Anchoring Single Ruthenium Sites

作者：Yang, Jian[1,4];Chen, Bingxu[2];Liu, Xiaokang[3];Liu, Wei[3];Li, Zhijun[1,4];Dong, Juncai[4,5,6];Chen, Wenxing[4,5,6];Yan, Wensheng[3];Yao, Tao[3];Duan, Xuezhi[2];Wu, Yuen[1,4];Li, Yadong[4]

机构：[1]Univ Sci & Technol China, Dept Chem, iChEM Collaborat Innovat Ctr Chem Energy Mat, Hefei 230026, Anhui, Peoples R China;[2]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China;[4]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China;[5]Beijing Inst Technol, Beijing Key Lab Construct Tailorable Adv Funct Ma, Sch Mat Sci & Engn, Beijing 100081, Peoples R China;[6]Inst High Energy Phys, Beijing 100029, Peoples R China

年份：2018

卷号：57

期号：30

起止页码：9495

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20182905575612);WOS:【SCI-EXPANDED(收录号:WOS:000438712600050)】；

基金：This work was supported by National Key R&D Program of China 2017YFA (0208300, 0700100), and the National Natural Science Foundation of China (21522107, 21671180, 21521091, U1463202). We thank the photoemission end-stations BL1W1B in Beijing Synchrotron Radiation Facility (BSRF), BL14W1 in Shanghai Synchrotron Radiation Facility (SSRF), BL10B and BL11U in National Synchrotron Radiation Laboratory (NSRL), for the help with characterization.

语种：英文

外文关键词：carbon-free supports; hydrogen evolution reaction (HER); phosphorus nitride; ruthenium; single atoms

摘要：Amorphous phosphorus nitride imide nanotubes (HPN) are reported as a novel substrate to stabilize materials containing single-metal sites. Abundant dangling unsaturated P vacancies play a role in stabilization. Ruthenium single atoms (SAs) are successfully anchored by strong coordination interactions between the d orbitals of Ru and the lone pair electrons of N located in the HPN matrix. The atomic dispersion of Ru atoms can be distinguished by X-ray absorption fine structure measurements and spherical aberration correction electron microscopy. Importantly, RuSAs@PN is an excellent electrocatalyst for the hydrogen evolution reaction (HER) in 0.5 M H2SO4, delivering a low overpotential of 24 mV at 10 mA cm(-2) and a Tafel slope of 38 mV dec(-1). The catalyst exhibits robust stability in a constant current test at a large current density of 162 mA cm(-2) for more than 24 hours, and is operative for 5000 cycles in a cyclic voltammetry test. Additionally, RuSAs@PN presents a turnover frequency (TOF) of 1.67 H(2)s(-1) at 25 mV, and 4.29 H(2)s(-1) at 50 mV, in 0.5 M H2SO4 solution, outperforming most of the reported hydrogen evolution catalysts. Density functional theory (DFT) calculations further demonstrate that the Gibbs free energy of adsorbed H* over the Ru SAs on PN is much closer to zero compared with the Ru/C and Ru SAs supported on carbon and C3N4, thus considerably facilitating the overall HER performance.