Cooperative copper centres in a metal-organic framework for selective conversion of CO2 to ethanol

被引：328

作者：

An, Bing ^{[1
]}

Li, Zhe ^{[1
]}

Song, Yang ^{[2
]}

Zhang, Jingzheng ^{[1
]}

Zeng, Lingzhen ^{[1
]}

Wang, Cheng ^{[1
]}

Lin, Wenbin ^{[1
,2
]}

机构：

[1] Xiamen Univ, Coll Chem & Chem Engn, Dept Chem, Collaborat Innovat Ctr Chem Energy Mat,State Key, Xiamen, Fujian, Peoples R China

[2] Univ Chicago, Dept Chem, 5735 S Ellis Ave, Chicago, IL 60637 USA

来源：

NATURE CATALYSIS | 2019年 / 2卷 / 08期

基金：

中国国家自然科学基金;

关键词：

HIGHLY-ACTIVE HYDROGENATION; SECONDARY BUILDING UNITS; HIGHER ALCOHOL SYNTHESIS; SITE COBALT CATALYSTS; CU/ZNO/AL2O3; CATALYSTS; CARBON-DIOXIDE; METHANOL; SYNGAS; ENERGY; NODES;

D O I：

10.1038/s41929-019-0308-5

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Selective conversion of CO2 to ethanol is of great interest but presents a significant challenge in forming a C-C bond while keeping a C-O bond intact throughout the process. Here, we report cooperative Cu-I sites on a Zr-12 cluster of a metal-organic framework (MOF) for selective hydrogenation of CO2 to ethanol. With the assistance of an alkali cation, the spatially proximate Zr-12-supported Cu-I centres activate hydrogen via bimetallic oxidative addition and promote C-C coupling to produce ethanol. The Cs+-modified MOF catalyst, in 10 hours, produces ethanol with >99% selectivity and a turnover number (based on all Cu atoms) of 4,080 in supercritical CO2, with 30 MPa of CO2 and 5 MPa of H-2 at 85 degrees C, or a turnover number of 490 at 2 MPa of CO2/H-2 (1/3) and 100 degrees C. Our work highlights the potential of using MOFs as a tunable platform to design earth-abundant metal catalysts for CO2 conversion.

引用

页码：709 / 717

页数：9

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[1] Challenges in the Greener Production of Formates/Formic Acid, Methanol, and DME by Heterogeneously Catalyzed CO2 Hydrogenation Processes [J].