CO2 Hydrogenation to Formate and Formic Acid by Bimetallic Palladium-Copper Hydride Clusters

被引：98

作者：

Liu, Gaoxiang ^{[1
]}

Poths, Patricia ^{[2
]}

Zhang, Xinxing ^{[3
]}

Zhu, Zhaoguo ^{[1
]}

Marshall, Mary ^{[1
]}

Blankenhorn, Moritz ^{[1
]}

Alexandrova, Anastassia N. ^{[2
]}

Bowen, Kit H. ^{[1
]}

机构：

[1] Johns Hopkins Univ, Dept Chem, Baltimore, MD 21218 USA

[2] Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA

[3] Nankai Univ, Coll Chem, Renewable Energy Convers & Storage Ctr ReCAST, Key Lab Adv Energy Mat Chem,Minist Educ, Tianjin 300071, Peoples R China

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2020年 / 142卷 / 17期

基金：

国家重点研发计划;

关键词：

CARBON-DIOXIDE; CO2; ACTIVATION; AB-INITIO; CU; PHOTOELECTRON; HYDROGENATION; ANIONS; DEHYDROGENATION; REDUCTION; COMPLEXES;

D O I：

10.1021/jacs.0c01855

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Mass spectrometric analysis of the anionic products of interaction between bimetallic palladium-copper tetrahydride anions, PdCuH4-, and carbon dioxide, CO2, in a reaction cell shows an efficient generation of the PdCuCO(2)H4(-) intermediate and formate/formic acid complexes. Multiple structures of PdCuH4- and PdCuCO2H4- are identified by a synergy between anion photoelectron spectroscopy and quantum chemical calculations. The higher energy PdCuH4- isomer is shown to drive the catalytic hydrogenation of CO2, emphasizing the importance of accounting for higher energy isomers for cluster catalytic activity. This study represents the first example of CO2 hydrogenation by bimetallic hydride clusters.

引用

页码：7930 / 7936

页数：7

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