Harnessing Electrocatalytic Coupling of Carbon Dioxide and Methanol for High‐Efficiency Formic Acid Production

作者：Zhikeng Zheng, Xiaobo Zheng, Ligang Wang, Huiming Wen, Ke Li, Zhenhao Xu, Yameng Fan, Peng Li, Suyu Zhang, Bin Liu, Dingsheng S. Wang, Kai Yan, Guoxiu Wang · 发表于：Angewandte Chemie International Edition · 年份：2025 · DOI：10.1002/anie.202512078 · 被引用次数：32 · 研究领域：CO2 Reduction Techniques and Catalysts、Carbon dioxide utilization in catalysis、Ionic liquids properties and applications

Abstract The coupling of electrocatalytic CO 2 reduction (ECR) and methanol oxidation reaction (MOR) presents a promising strategy for simultaneous cogeneration of formic acid (FA) at both cathode and anode. However, sluggish kinetics, low selectivity and efficiency hinder practical application. Herein, we demonstrate an integrated ECR||MOR system employing CuBi cathode and NiCo anode for energy‐efficient FA cogeneration. The CuBi alloy achieves high Faradaic efficiencies (FE > 90%) for FA generation over an extensive potential range (>400 mV), attributed to the accelerated formation of HCOO * intermediates in facilitating FA production. Meanwhile, the NiCo alloy reached a remarkable FE of 97.5% for FA generation at 1.4 V versus reversible hydrogen electrode, benefiting from rapid HCOO * intermediate formation that effectively mitigates CO toxicity. This unique system delivered a current density of 10 mA cm −2 at a voltage of 2.07 V, representing a substantial reduction of 320 mV compared to water electrolysis. Across a wide operational voltage window (2.0–2.8 V), the system consistently delivered total Faradaic efficiencies ranging between 189% and 192%, alongside exceptional FA production capacities surpassing 400 g kWh −1 , which significantly outperformed traditional methods (∼220 g kWh −1 ). This work provides an efficient pathway for low‐energy CO 2 utilization and sustainable FA production.