文献类型：期刊文献

英文题名：Taming Electrons in Pt/C Catalysts to Boost the Mesokinetics of Hydrogen Production

作者：Chen, Wenyao[1];Fu, Wenzhao[1];Duan, Xuezhi[1];Chen, Bingxu[1];Qian, Gang[1];Si, Rui[2];Zhou, Xinggui[1];Yuan, Weikang[1];Chen, De[3]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[3]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2022

卷号：14

起止页码：124

外文期刊名：ENGINEERING

收录：;EI(收录号：20222712317668);WOS:【SCI-EXPANDED(收录号:WOS:000864881600018)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803, 92034301, 22008066, and 21776077), the China Postdoctoral Science Foundation (BX20190116), the Innovation Program of Shanghai Municipal Education Commission, the Program of Shanghai Academic/Technology Research Leader (21XD1421000), 111 Project of the Ministry of Education of China (B08021). The authors thank beamline BL14W1 (Shanghai Synchrotron Radiation Facility) for the beam time and assistant in the experiments.

语种：英文

外文关键词：Mesokinetics model; Catalyst descriptor; Pt charge state; Carbon surface chemistry; Hydrogen generation activity

摘要：Taming the electron transfer across metal-support interfaces appears to be an attractive yet challenging methodology to boost catalytic properties. Herein, we demonstrate a precise engineering strategy for the carbon surface chemistry of Pt/C catalysts-that is, for the electron-withdrawing/donating oxygen -containing groups on the carbon surface-to fine-tune the electrons of the supported metal nanoparticles. Taking the ammonia borane hydrolysis as an example, a combination of density functional theory (DFT) calculations, advanced characterizations, and kinetics and isotopic analyses reveals quantifiable relation-ships among the carbon surface chemistry, Pt charge state and binding energy, activation entropy/ enthalpy, and resultant catalytic activity. After decoupling the influences of other factors, the Pt charge is unprecedentedly identified as an experimentally measurable descriptor of the Pt active site, contribut-ing to a 15-fold increment in the hydrogen generation rate. Further incorporating the Pt charge with the number of Pt active sites, a mesokinetics model is proposed for the first time that can individually quantify the contributions of the electronic and geometric properties to precisely predict the catalytic performance. Our results demonstrate a potentially groundbreaking methodology to design and manip-ulate metal-carbon catalysts with desirable properties.(c) 2022 THE AUTHORS. Published by Elsevier LTD on behalf of Chinese Academy of Engineering and Higher Education Press Limited Company. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).