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Lecture Time:2026-01-15

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Recently, the Cluster Molecular Materials Research Team within the School of Chemistry and Materials Science at Hebei Normal University has made a significant breakthrough in the field of electrocatalysis based on metal-organic frameworks (MOFs). The related research findings were published under the title "Regulation of the D-Band Center Through Ligand Engineering in Silver Cluster-Based MOFs Enhances Acidic CO2 Electroreduction" in Angewandte Chemie International Edition, a top-tier international journal in the field of chemistry. Hebei Normal University is the sole completing institution for this paper. Dr. Liu Yuanyuan, a young faculty member of the School of Chemistry and Materials Science, serves as the first author, while Professor Zhao Xiaojia and Professor Han Zhangang are the co-corresponding authors.

Utilizing intermittent renewable energy to convert CO2 into high-value chemicals and fuels via electrochemical reduction (CO2RR) is a highly cutting-edge research topic. This reaction heavily relies on electrocatalysts that possess ultra-high activity, selectivity, and stability. To address this challenge, the research team proposed a "ligand engineering" strategy: using Ag12 clusters as metal nodes, they constructed silver cluster-based MOF structures with tunable coordination microenvironments by introducing ligands with different electronic properties. This approach achieved precise regulation of the d-band center of the metal sites. The resulting catalyst demonstrated excellent electrocatalytic activity for CO2 reduction under acidic conditions, with no significant performance degradation after 70 hours of continuous operation.

The study reveals that the strong Lewis basicity and σ-electron-donating ability of imidazole ligands significantly upshift the d-band center of the Ag12 clusters. This optimizes the adsorption of the key intermediate *COOH and lowers the reaction energy barrier, thereby enabling efficient and highly selective reduction of CO2 to CO in strongly acidic environments. The research elucidates the structure-activity relationship between the electronic structure of organic ligands and electrocatalytic performance, providing new insights and strategies for designing and developing high-performance acidic CO2 reduction electrocatalysts with practical application value.

This work was supported by projects including the National Natural Science Foundation of China and the Natural Science Foundation of Hebei Province.

Paper Link: https://doi.org/10.1002/anie.202518779