A highly CO-tolerant atomically dispersed Pt catalyst for chemoselective hydrogenation

被引:345
作者
Lin, Lili [1 ,2 ]
Yao, Siyu [1 ,2 ]
Gao, Rui [3 ,4 ,5 ]
Liang, Xuan [1 ,2 ]
Yu, Qiaolin [1 ,2 ]
Deng, Yuchen [1 ,2 ]
Liu, Jinjia [3 ,4 ]
Peng, Mi [1 ,2 ]
Jiang, Zheng [6 ]
Li, Siwei [1 ,2 ]
Li, Yong-Wang [3 ,4 ]
Wen, Xiao-Dong [3 ,4 ,7 ]
Zhou, Wu [8 ,9 ]
Ma, Ding [1 ,2 ]
机构
[1] Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, Coll Engn, Beijing, Peoples R China
[2] Peking Univ, BIC ESAT, Beijing, Peoples R China
[3] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan, Shanxi, Peoples R China
[4] Synfuels China Co Ltd, Natl Energy Ctr Coal Liquids, Beijing, Peoples R China
[5] Inner Mongolia Univ, Sch Chem & Chem Engn, Hohhot, Peoples R China
[6] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai, Peoples R China
[7] Ind Univ Cooperat Base Beijing Informat S & TUniv, Beijing Adv Innovat Ctr Mat Genome Engn, Beijing, Peoples R China
[8] Univ Chinese Acad Sci, Sch Phys Sci, Beijing, Peoples R China
[9] Univ Chinese Acad Sci, CAS Ctr Excellence Topol Quantum Computat, Beijing, Peoples R China
基金
国家重点研发计划;
关键词
TOTAL-ENERGY CALCULATIONS; CARBON-MONOXIDE; SELECTIVE HYDROGENATION; NITRO-COMPOUNDS; GOLD; SINGLE; OXIDATION; PLATINUM; ATOM; NITROAROMATICS;
D O I
10.1038/s41565-019-0366-5
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
The hydrogenation activity of noble metal, especially platinum (Pt), catalysts can be easily inhibited by the presence of a trace amount of carbon monoxide (CO) in the reaction feeds. Developing CO-resistant hydrogenation catalysts with both high activity and selectivity is of great economic interest for industry as it allows the use of cheap crude hydrogen and avoids costly product separation. Here we show that atomically dispersed Pt over alpha-molybdenum carbide (alpha-MoC) constitutes a highly CO-resistant catalyst for the chemoselective hydrogenation of nitrobenzene derivatives. The Pt-1/alpha-MoC catalyst shows promising activity in the presence of 5,000 ppm CO, and has a strong chemospecificity towards the hydrogenation of nitro groups. With the assistance of water, high hydrogenation activity can also be achieved using CO and water as a hydrogen source, without sacrificing selectivity and stability. The weakened CO binding over the electron-deficient Pt single atom and a new reaction pathway for nitro group hydrogenation confer high CO resistivity and chemoselectivity on the catalyst.
引用
收藏
页码:354 / +
页数:9
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