文献类型：期刊文献

英文题名：Atomic Insights into Robust Pt-PdO Interfacial Site-Boosted Hydrogen Generation

作者：Chen, Wenyao[1];Zheng, Weizhong[1];Cao, Junbo[1];Fu, Wenzhao[1];Qian, Gang[1];Chen, De[2];Zhou, Xinggui[1];Duan, Xuezhi[1]

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

年份：2020

卷号：10

期号：19

起止页码：11417

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20204709511313);WOS:【SCI-EXPANDED(收录号:WOS:000577156300049)】；

基金：This work was financially supported by the Natural Science Foundation of China (21922803 and 21776077), the China Postdoctoral Science Foundation (BX20190116), the Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning, the State Key Laboratory of Organic-Inorganic Composites (oic-201801007), 111 Project of the Ministry of Education of China (B08021), and the Open Project of State Key Laboratory of Chemical Engineering (SKLChe-15C03). The authors thank beamline BL14W1 (Shanghai Synchrotron Radiation Facility) for the beam time and assistance in the experiments.

语种：英文

外文关键词：Pt-PdO interfacial sites; atomic insights; hydrogen generation; activity and durability; volcano curve

摘要：Suppression of catalyst deactivation without compromising activity has been a long-standing yet elusive goal in heterogeneous catalysis. Herein, we report a remarkable achievement of both hydrogen generation activity and durability by atomically engineering Pt-PdO interfacial sites. A combination of kinetics (isotopic) analyses, multiple characterization techniques, molecular dynamics, and density functional theory calculations was employed to reveal the evolution of the Pt-Pd atomic structure where Pd segregates to the outer surface of Pt nanoparticles, followed by partial oxidation, resulting in the structure of a Pt-rich core and a PdO-Pd-rich shell. The strong capability of PdO to activate H2O compensates for its adverse effects on Pt electronic properties and creates the Pt and PdO interfacial sites for ammonia borane and H2O activation, respectively. Moreover, because of the strong electron repulsion and steric hindrance effects, these surface PdO sites strongly inhibit the adsorption of B(OH)(4)(-), thus protecting Pt active sites from poisoning. As a result, such a unique atomic structure with a Pt-Pd ratio of 1:1 is found to be the most promising catalyst at the apex of the volcano curve. The strategy developed here unambiguously clarifies the activity and durability attributes of Pt-PdO interfacial sites for this reaction and sheds light on the design of a new type of highly active yet stable metal catalysts.