Cation enrichment promotes high-rate CO electroreduction to C2+ liquid products

Cui, Chunyu, Xu, Liang, Yu, Peiping, Wang, Nan, Ni, Fenglou, Guo, Wen, Yang, Hao, Cheng, Tao and Zhang, Bo 2024. Cation enrichment promotes high-rate CO electroreduction to C2+ liquid products. Chemistry-Sustainability-Energy-Materials , e202400940. 10.1002/cssc.202400940 Item availability restricted.

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Abstract

Electrochemical reduction of CO into valuable multicarbon (C2+) liquids is crucial for reducing CO2 emissions and advancing clean energy, yet mastering efficiency and selectivity in this process remains a tough challenge. Herein, we employ a surface-modification strategy using electrochemically active polymeric 1,4,5,8-naphthalenete-tracarboxylic dianhydride (PNTCDA)-modified copper nanosheets (PM-Cu) to rearrange reactive species in the electric double layer, where the PNTCDA triggers a distinctive enolization that anchor potassium ions (K+) onto the cathode surface under reduction condition. Electrochemical analysis and computational simulations revealed that this approach fine-tunes K+ distribution in the double layer, making the dehydration of hydrated K+ more efficient and reducing active water molecules at the interface, thus inhibiting the hydrogen evolution reaction while concurrently promoting CO reduction via enhanced C‒C coupling. For the first time, the PM-Cu catalyst demonstrates ampere-scale current densities with the exclusive selectivity of a C2+ liquid product yield exceeding 90%. Thus, by tailoring the local microenvironment with electrochemically active organics, it is possible to modulate CO reduction, improve sustainable energy storage, and increase industrial carbon utilization.

Item Type:	Article
Date Type:	Published Online
Status:	In Press
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	Wiley
ISSN:	1864-5631
Date of First Compliant Deposit:	1 November 2024
Date of Acceptance:	21 August 2024
Last Modified:	06 Nov 2024 02:45
URI:	https://orca.cardiff.ac.uk/id/eprint/173595

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