Selective and Efficient CO Electroreduction to Formate on Copper Electrodes Modified by Cationic Gemini Surfactants.

Angew Chem Int Ed Engl

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Zhongguancun North First Street 2, Beijing, 100190, P. R. China.

Published: February 2024

Electroreduction of CO into valuable chemicals and fuels is a promising strategy to mitigate energy and environmental problems. However, it usually suffers from unsatisfactory selectivity for a single product and inadequate electrochemical stability. Herein, we report the first work to use cationic Gemini surfactants as modifiers to boost CO electroreduction to formate. The selectivity, activity and stability of the catalysts can be all significantly enhanced by Gemini surfactant modification. The Faradaic efficiency (FE) of formate could reach up to 96 %, and the energy efficiency (EE) could achieve 71 % over the Gemini surfactants modified Cu electrode. In addition, the Gemini surfactants modified commercial Bi O nanosheets also showed an excellent catalytic performance, and the FE of formate reached 91 % with a current density of 510 mA cm using the flow cell. Detailed studies demonstrated that the double quaternary ammonium cations and alkyl chains of the Gemini surfactants played a crucial role in boosting electroreduction CO , which can not only stabilize the key intermediate HCOO* but also provide an easy access for CO . These observations could shine light on the rational design of organic modifiers for promoted CO electroreduction.

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Source
http://dx.doi.org/10.1002/anie.202315822DOI Listing

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