文献类型：期刊文献

英文题名：Mechanistic and kinetic insights into the Pt-Ru synergy during hydrogen generation from ammonia borane over PtRu/CNT nanocatalysts

作者：Chen, Wenyao[1,2];Li, Dali[1];Peng, Chong[1];Qian, Gang[1];Duan, Xuezhi[1];Chen, De[2];Zhou, Xinggui[1]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway

年份：2017

卷号：356

起止页码：186

外文期刊名：JOURNAL OF CATALYSIS

收录：;EI(收录号：20174504364768);WOS:【SCI-EXPANDED(收录号:WOS:000418223300018)】；

基金：This work was financially supported by the Natural Science Foundation of China (21776077 and 21306046), the Shanghai Natural Science Foundation (17ZR1407300 and 17ZR1407500), the Shanghai Rising-Star Program (17QA1401200), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, Fundamental Research Funds for the Central Universities (222201718003 and YA0142125), the Open Project of State Key Laboratory of Chemical Engineering (SKL-Che-15C03), and the 111 Project of the Ministry of Education of China (B08021).

语种：英文

外文关键词：PtRu catalyst; Hydrogen generation; Activity and durability; Volcano curve; Kinetic and isotopic analyses

摘要：Increasing the utilization efficiency of noble metals by the synergy with less expensive metals is an important yet challenging issue in heterogeneous catalysis. Herein, exemplified with Pt-catalyzed hydrolytic dehydrogenation of ammonia borane, partial substitution of the Pt catalysts by over 11 times less expensive Ru is studied to obtain highly efficient and cost-effective Pt-based catalysts. It is observed that the Pt-Ru bimetallic catalysts, especially Pt0.5Ru0.5/CNT, deliver higher hydrogen generation activity and durability than the Pt/CNT and Ru/CNT catalysts, indicating a remarkable Pt-Ru synergy. The underlying nature of this synergy is elucidated by combining kinetic and isotopic analyses with multiple techniques such as HAADF-STEM, EDX, XRD, H-2-TPR, HRTEM, XPS and ICP-AES. The appropriate activation energy and entropy of activation for the reaction are mainly responsible for the highly active Pt0.5Ru0..5/CNT catalyst, and a volcano-shaped relationship for the reactivity of these five catalysts as a function of entropy of activation is proposed. The insights revealed here might guide the rational design of catalysts for this reaction, and the methodology could be extended to unravel the nature of other bi- or multi-metallic catalysts. (C) 2017 Elsevier Inc. All rights reserved.