Polymeric ionic liquid promotes acidic electrocatalytic CO<sub>2</sub> conversion to multicarbon products with ampere level current on Cu.

Tan, Zhonghao; Zhang, Jianling; Yang, Yisen; Zhong, Jiajun; Zhao, Yingzhe; Teng, Yunan; Han, Buxing; Chen, Zhongjun · Nat Commun · 2025

basic_science · Level V

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Abstract

The acidic electroreduction of CO<sub>2</sub> into multicarbon (C<sub>2+</sub>) products is much attractive for the improved carbon utilization than alkaline or neutral electroreduction. How to improve the efficiency of C<sub>2+</sub> products generation by acidic electroreduction of CO<sub>2</sub>, is important, especially at high current density and in electrolyte with low K<sup>+</sup> concentration. Herein, we propose a strategy of capping Cu surface with a polymeric ionic liquid (PIL) adlayer for boosting the acidic electrocatalytic CO<sub>2</sub> conversion to C<sub>2+</sub> products at high current densities (ampere-level) and low K<sup>+</sup> concentration. In the electrolyte with a relatively low K<sup>+</sup> concentration (1.0 M), the Faradaic efficiency (FE) for C<sub>2+</sub> products reaches 82.2% under a current density 1.0 A·cm<sup>-2</sup> in acidic environment (pH=1.8). Particularly, when the current density is as high as 1.5 A·cm<sup>-2</sup>, the C<sub>2+</sub> FE still keeps 75.8%. Experimental and theoretical studies reveal that the presence of PIL adlayer on Cu catalyst can well inhibit H<sup>+</sup> diffusion to catalyst surface, enrich more K<sup>+</sup> and facilitate C-C coupling reaction.