Abstract

The electrochemical carbon dioxide reduction reaction to syngas with controlled CO/H2 ratios has been studied on Pd-based bimetallic hydrides using a combination of in situ characterization and density functional theory calculations. When compared with pure Pd hydride, the bimetallic Pd hydride formation occurs at more negative potentials for Pd-Ag, Pd-Cu, and Pd-Ni. Theoretical calculations show that the choice of the second metal has a more significant effect on the adsorption strength of *H than *HOCO, with the free energies between these two key intermediates (i.e., ΔG(*H)–ΔG(*HOCO)) correlating well with the carbon dioxide reduction reaction activity and selectivity observed in the experiments, and thus can be used as a descriptor to search for other bimetallic catalysts. The results also demonstrate the possibility of alloying Pd with non-precious transition metals to promote the electrochemical conversion of CO2 to syngas.

Details

Title
Tuning the activity and selectivity of electroreduction of CO2 to synthesis gas using bimetallic catalysts
Author
Lee, Ji Hoon 1 ; Kattel, Shyam 2 ; Zhao, Jiang 3 ; Xie, Zhenhua 4 ; Yao, Siyu 5 ; Tackett, Brian M 1 ; Xu, Wenqian 6 ; Marinkovic, Nebojsa S 4 ; Chen, Jingguang G 4 

 Department of Chemical Engineering, Columbia University, New York, NY, USA 
 Department of Physics, Florida A&M University, Tallahassee, FL, USA 
 Department of Chemical Engineering, School of Chemical Engineering and Technology, Xi’an Jiaotong University, Xi’an, Shaanxi, P. R. China 
 Department of Chemical Engineering, Columbia University, New York, NY, USA; Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA 
 Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA 
 X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, IL, USA 
Pages
1-8
Publication year
2019
Publication date
Aug 2019
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
2275917135
Copyright
© 2019. 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.