Molecular-Level Insights into the Notorious CO Poisoning of Platinum Catalyst

被引：100
作者：
Chen, Wenyao [1 ]
Cao, Junbo [1 ]
Fu, Wenzhao [1 ]
Zhang, Jing [1 ]
Qian, Gang [1 ]
Yang, Jia [2 ]
Chen, De [2 ]
Zhou, Xinggui [1 ]
Yuan, Weikang [1 ]
Duan, Xuezhi [1 ]
机构：
[1] East China Univ Sci & Technol, Sch Chem Engn, State Key Lab Chem Engn, Shanghai 200237, Peoples R China
[2] Norwegian Univ Sci & Technol, Dept Chem Engn, N-7491 Trondheim, Norway
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 16期
基金：
中国博士后科学基金;
关键词：
Activation; Adsorption; CO Poisoning; Electrons; Kinetics; SINGLE-ATOM; ELECTRONIC-PROPERTIES; SELECTIVE OXIDATION; CERIA; ZINC;
D O I：
10.1002/anie.202200190
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Carbon monoxide (CO) is notorious for its strong adsorption to poison platinum group metal catalysts in the chemical industry. Here, we conceptually distinguish and quantify the effects of the occupancy and energy of d electrons, emerging as the two vital factors in d-band theory, for CO poisoning of Pt nanocatalysts. The stepwise defunctionalization of carbon support is adopted to fine-tune the 5d electronic structure of supported Pt nanoparticles. Excluding other promotional mechanisms, the increase of Pt 5d band energy strengthens the competitive adsorption of hydrogen against CO for the preferential oxidation of CO, affording the scaling relationship between Pt 5d band energy and CO/H-2 adsorption energy difference. The decrease of Pt 5d band occupancy lowers CO site coverage to promote its association with oxygen for the total oxidation of CO, giving the scaling relationship between Pt 5d occupancy and activation energy. The above insights outline a molecular-level understanding of CO poisoning.
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页数：9
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