Unraveling the rate-limiting step of two-electron transfer electrochemical reduction of carbon dioxide

Wanyu Deng, Peng Zhang, Brian Seger () and Jinlong Gong ()
Additional contact information
Wanyu Deng: Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Peng Zhang: Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)
Brian Seger: Technical University of Denmark
Jinlong Gong: Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin)

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract Electrochemical reduction of CO2 (CO2ER) has received significant attention due to its potential to sustainably produce valuable fuels and chemicals. However, the reaction mechanism is still not well understood. One vital debate is whether the rate-limiting step (RLS) is dominated by the availability of protons, the conversion of water molecules, or the adsorption of CO2. This paper describes insights into the RLS by investigating pH dependency and kinetic isotope effect with respect to the rate expression of CO2ER. Focusing on electrocatalysts geared towards two-electron transfer reactions, we find the generation rates of CO and formate to be invariant with either pH or deuteration of the electrolyte over Au, Ag, Sn, and In. We elucidate the RLS of two-electron transfer CO2ER to be the adsorption of CO2 onto the surface of electrocatalysts. We expect this finding to provide guidance for improving CO2ER activity through the enhancement of the CO2 adsorption processes by strategies such as surface modification of catalysts as well as careful control of pressure and interfacial electric field within reactors.

Date: 2022
References: View complete reference list from CitEc
Citations: View citations in EconPapers (7)

Downloads: (external link)
https://www.nature.com/articles/s41467-022-28436-z 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:13:y:2022:i:1:d:10.1038_s41467-022-28436-z

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

DOI: 10.1038/s41467-022-28436-z

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 ().