Recently, the research team led by Professor Shimou Chen and Associate Professor Ying Xiao from the School of Materials Science and Engineering published a research paper titled Electronic Localization Modulation of the Cyano-Bridged Cu₃[Co(CN)₆]₂ Catalyst with Heterometallic Active Sites for High-Performance Li-CO₂ Batteries in Advanced Energy Materials. This study constructed a cyano-bridged Cu₃[Co(CN)₆]₂ catalyst featuring heterometallic active sites, which enhances the kinetics of CO₂ conversion reactions through electronic localization modulation, significantly extending the cycle life of Li-CO₂ batteries.
Li-CO₂ batteries exhibit an ultrahigh energy density of 1876 Wh kg⁻¹, making them promising power sources for portable electronics and electric vehicles while enabling efficient conversion and utilization of the greenhouse gas CO₂. However, sluggish reaction kinetics at the gas-liquid-solid triple-phase interfaces during electrochemical processes leads to high overpotentials and limited cycle life, severely hindering their development and practical application. To address this, this work constructed a CN⁻-modulated CoCu bimetallic active site cathode catalyst (denoted CoCuCN) and elucidated its microscopic mechanism for enhancing Li-CO₂ battery performance. The mixed-valence metal structure formed by CN⁻ bridging exhibits asymmetric electron distribution characteristics, facilitating unique electron transfer processes. The CoCu bimetallic active sites establish dynamic electronic equilibrium through CN⁻-mediated electronic coupling, optimizing electron distribution across different reaction stages. Benefiting from this distinctive local structural modulation, the CoCuCN-catalyzed Li-CO₂ batteries demonstrate ultra-stable cycling (over 1480 hours) with an ultralow overpotential of 1.18 V at 300 mA g⁻¹. This work provides new insights for designing low-cost bimetallic site catalysts for advanced Li-CO₂ batteries.
The first author is Shilin Hu (2022 Master's candidate), with co-corresponding authors Prof. Shimou Chen and Assoc. Prof. Ying Xiao from Beijing University of Chemical Technology. Beijing University of Chemical Technology is the primary affiliation. This research was supported by the National Natural Science Foundation of China and the Fundamental Research Funds for the Central Universities.
The link to the paper is:
https://advanced.onlinelibrary.wiley.com/doi/full/10.1002/aenm.202501001
