Electronic Localization Modulation of the Cyano‐Bridged Cu 3 [Co(CN) 6 ] 2 Catalyst With Heterometallic Active Sites for High‐Performance Li‐CO 2 Batteries

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Abstract
Lithium‐carbon dioxide (Li‐CO 2 ) batteries represent an emerging and promising technology that combines energy storage with environmental sustainability by effectively capturing and converting CO 2 . However, the sluggish electrochemical reaction kinetics and excessive accumulation of the discharge product with low conductivity at the cathode always lead to large polarization and limited lifespan of the battery. Herein, a new cyano‐bridged heterometallic active site catalyst (Cu 3 [Co(CN) 6 ] 2 ) is proposed to augment CO 2 transformation reaction kinetics through electronic localization modulation. Computational simulation and series experiments confirm that the asymmetric electronic distribution in the cyano‐bridge promotes distinct electron transfer, which significantly improves the CO 2 adsorption ability and catalytic activity of the Co active site with the assistance of the Cu active site, contributing to a remarkable efficiency in driving the CO 2 reduction and simultaneously facilitates CO 2 evolution reactions. Consequently, the assembled Li‐CO 2 batteries manifest attractive cycling stability exceeding 1480 h with a low overpotential of 1.18 V at 300 mA g −1 , exhibiting appealing competition with the previously reported work. This work offers an ingenious insight into designing low‐cost dual‐metal site catalysts for advanced Li‐CO 2 batteries.
Funding Information
  • Fundamental Research Funds for the Central Universities (buctrc202104)
  • Fundamental Research Funds for the Central Universities (buctrc202114)
  • National Natural Science Foundation of China (U24A20566)
  • National Natural Science Foundation of China (52302210)
  • National Natural Science Foundation of China (52425207)

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