Redox-Mediated Ligand Exfoliation Enables High-Density Single-Site Molecular Catalysts for CO₂ Electroreduction.

Authors

Yanjie Fang, Yifan Gao, Feiqing Sun, Feiyang Hong, Bing Shan

Published in

Small (Weinheim an der Bergstrasse, Germany). Pages e75271. Aug 17, 2026. Epub Aug 17, 2026.

Abstract

Conventional strategies for fabricating single-site electrocatalysts often suffer from metal aggregation and insufficient exposure of active sites, limiting their efficiency in CO₂ electroreduction. Here we present a redox-mediated ligand exfoliation method to construct single-site molecular catalysts with high-density, atomically dispersed active sites in a conductive polymer network. Through tailored integration of molecular assemblies and subsequent reductive cleavage of axially coordinated ligands, coordinatively unsaturated metal sites are exposed on the electrode surface. This architecture enhances CO₂ adsorption and activation, facilitating synergistic CO₂-to-CO conversion at cobalt sites and subsequent CO-to-methanol transformation at adjacent copper sites. The optimized catalyst achieves a methanol production rate of 9.2 mol h^-1 g^-1 with partial current density of 142 mA cm^-2. In situ spectroscopic and theoretical analyses elucidate the critical role of site exposure in the enhanced activity. This work establishes a generalizable pathway to address the limitations of traditional single-site catalysts in designing electrocatalysts with enhanced site exposure and stability.

PMID:
42605578
Bibliographic data and abstract were imported from PubMed on 17 Aug 2026.

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