Abstract

Catalytic transformation of CO2 to formate is generally realized through bicarbonate hydrogenation in an alkaline environment, while it suffers from a thermodynamic sink due to the considerable thermodynamic stability of the bicarbonate intermediate. Here, we devise a route for the direct catalytic conversion of CO2 over a Schiff-base-modified gold nanocatalyst that is comparable to the fastest known nanocatalysts, with a turnover number (TON) of up to 14,470 over 12 h at 90 °C. Theoretical calculations and spectral analysis results demonstrate that the activation of CO2 can be achieved through a weakly bonded carbamate zwitterion intermediate derived from a simple Lewis base adduct of CO2. However, this can only occur with a hydrogen lacking Lewis base center in a polar solvent. This finding offers a promising avenue for the direct activation of CO2 and is likely to have considerable implications in the fields of CO2 conversion and gold catalytic chemistry.

Details

Title
Direct catalytic hydrogenation of CO2 to formate over a Schiff-base-mediated gold nanocatalyst
Author
Liu, Qinggang 1 ; Yang, Xiaofeng 2 ; Li, Lin 2 ; Miao, Shu 2 ; Li, Yong 3 ; Li, Yanqin 4 ; Wang, Xinkui 4 ; Huang, Yanqiang 2 ; Zhang, Tao 2 

 State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, Dalian, China; Dalian Institute of Chemical Physics, Collaborative Innovation Center of Chemistry for Energy Materials, Chinese Academy of Sciences, Dalian, China 
 Dalian Institute of Chemical Physics, Collaborative Innovation Center of Chemistry for Energy Materials, Chinese Academy of Sciences, Dalian, China 
 Institute of Applied and Physical Chemistry and Center for Environmental Research and Sustainable Technology, University of Bremen, Bremen, Germany 
 State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, Dalian, China 
Pages
1-8
Publication year
2017
Publication date
Nov 2017
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
1962261235
Copyright
© 2017. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.