DOI: 10.1002/ange.202317512 ISSN: 0044-8249

Accelerating the Reaction Kinetics of CO2 Reduction to MultiCarbon Products by Synergistic Effect between Cation and Aprotic Solvent on Copper Electrodes

Xiaowan Bai, Chaojie Chen, Xunhua Zhao, Yehui Zhang, Yao Zheng, Yan Jiao
  • General Medicine

Improving the selectivity of electrochemical CO2 reduction to multi‐carbon products (C2+) is an important and highly challenging topic. In this work, we propose and validate an effective strategy to improve C2+ selectivity on Cu electrodes, by introducing synergistic effect between cation (Na+) and aprotic solvent (DMSO) to the electrolyte. Based on constant potential ab initio molecular dynamics simulations, we first revealed that Na+ facilitates C‐C coupling while inhibits CH3OH/CH4 products via reducing the water network connectivity near the electrode. Furthermore, the water network connectivity was further decreased by introducing an aprotic solvent DMSO, leading to suppression of both C1 production and hydrogen evolution reaction with minimal effect on *OCCO* hydrogenation. The synergistic effect enhancing C2 selectivity was also experimentally verified through electrochemical measurements. The results showed that the Faradaic efficiency of C2 increases from 9.3% to 57% at 50 mA/cm2 under a mixed electrolyte of NaHCO3 and DMSO compared to a pure NaHCO3, which can significantly enhance the selectivity of the C2 product. Therefore, our discovery provides an effective electrolyte‐based strategy for tuning CO2RR selectivity through modulating the microenvironment at the electrode‐electrolyte interface.

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