Stable, active CO2 reduction to formate via redox-modulated stabilization of active sites

Le Li, Adnan Ozden, Shuyi Guo, F. Pelayo Garcı́a de Arquer, Chuanhao Wang, Mingzhe Zhang, Jin Zhang, Haoyang Jiang, Wei Wang, Hao Dong (), David Sinton, Edward H. Sargent () and Miao Zhong ()
Additional contact information
Le Li: Nanjing University
Adnan Ozden: University of Toronto
Shuyi Guo: Nanjing University
F. Pelayo Garcı́a de Arquer: University of Toronto
Chuanhao Wang: Nanjing University
Mingzhe Zhang: Nanjing University
Jin Zhang: Nanjing University
Haoyang Jiang: Nanjing University
Wei Wang: Nanjing University
Hao Dong: Nanjing University
David Sinton: University of Toronto
Edward H. Sargent: University of Toronto
Miao Zhong: Nanjing University

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract Electrochemical reduction of CO2 (CO2R) to formic acid upgrades waste CO2; however, up to now, chemical and structural changes to the electrocatalyst have often led to the deterioration of performance over time. Here, we find that alloying p-block elements with differing electronegativities modulates the redox potential of active sites and stabilizes them throughout extended CO2R operation. Active Sn-Bi/SnO2 surfaces formed in situ on homogeneously alloyed Bi0.1Sn crystals stabilize the CO2R-to-formate pathway over 2400 h (100 days) of continuous operation at a current density of 100 mA cm−2. This performance is accompanied by a Faradaic efficiency of 95% and an overpotential of ~ −0.65 V. Operating experimental studies as well as computational investigations show that the stabilized active sites offer near-optimal binding energy to the key formate intermediate *OCHO. Using a cation-exchange membrane electrode assembly device, we demonstrate the stable production of concentrated HCOO– solution (3.4 molar, 15 wt%) over 100 h.

Date: 2021
References: Add references at CitEc
Citations: View citations in EconPapers (4)

Downloads: (external link)
https://www.nature.com/articles/s41467-021-25573-9 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25573-9

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-021-25573-9

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().