Oxygen-tolerant CO<sub>2</sub> electroreduction over covalent organic frameworks via photoswitching control oxygen passivation strategy.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38368417.
- Also identified by DOI 10.1038/s41467-024-45959-9 and PMC identifier 10874412.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
The direct use of flue gas for the electrochemical CO<sub>2</sub> reduction reaction is desirable but severely limited by the thermodynamically favorable oxygen reduction reaction. Herein, a photonicswitching unit 1,2-Bis(5'-formyl-2'-methylthien-3'-yl)cyclopentene (DAE) is integrated into a cobalt porphyrin-based covalent organic framework for highly efficient CO<sub>2</sub> electrocatalysis under aerobic environment. The DAE moiety in the material can reversibly modulate the O<sub>2</sub> activation capacity and electronic conductivity by the framework ring-closing/opening reactions under UV/Vis irradiation. The DAE-based covalent organic framework with ring-closing type shows a high CO Faradaic efficiency of 90.5% with CO partial current density of -20.1 mA cm<sup>-2</sup> at -1.0 V vs. reversible hydrogen electrode by co-feeding CO<sub>2</sub> and 5% O<sub>2</sub>. This work presents an oxygen passivation strategy to realize efficient CO<sub>2</sub> electroreduction performance by co-feeding of CO<sub>2</sub> and O<sub>2</sub>, which would inspire to design electrocatalysts for the practical CO<sub>2</sub> source such as flue gas from power plants or air.