近日，华东师范大学汤静团队研究了调节界面电场作用下自演化串联催化剂对CO₂电还原的行为调控。该项研究成果发表在2025年8月19日出版的《德国应用化学》杂志上。

串联或自进化Cu基催化剂有效调节*CO，促进CO₂电还原转化为多碳（C₂₊）产物。DFT计算结果表明，Cu、Ag/Cu、Pd/Cu和Au/Cu模型在不同界面电场强度下对*CO的吸附能力不同。

因此，研究组设计了三种自进化串联催化剂，并研究了*CO在界面电场作用下的吸附和迁移行为。电化学CO₂还原实验结果表明，Au/Cu具有较高的CO选择性是由于其较弱的*CO吸附能力，原位衰减全反射-红外和原位拉曼光谱证实了这一点。

Pd/Cu的低C₂₊选择性是由于其高反应能垒和低催化活性。相比之下，Ag/Cu的FEC₂₊达到89.2%，偏电流密度（jc2+）为553.9 mA cm^-2，反应能垒低，CO吸附能力适中。COMSOL多物理场模拟表明，在纳米范围内，界面电场对*CO外迁移的影响可以忽略不计。虽然强大的界面电场增加了*CO内部迁移的能垒，但在富*CO微环境中，*CO的增强吸附能力仍然比串联催化剂主导着C-C耦合。

附：英文原文

Title: Behavior Regulation of *CO over Self-Evolution Tandem Catalysts Under Tuned Interfacial Electric Field Boosts CO2 Electroreduction

Author: Zining Zhang, Xinyan Ma, Yang Song, Xue Yang, Qi Fang, Yusuke Yamauchi, Jing Tang

Issue&Volume: 2025-08-19

Abstract: Tandem or self-evolution Cu-based catalysts effectively regulate *CO to promote the conversion of CO2 electroreduction to multicarbon (C2+) products. DFT calculations reveal that the adsorption capacity of *CO varies under different interfacial electric field intensities for the Cu, Ag/Cu, Pd/Cu, and Au/Cu models. Accordingly, we design three kinds of self-evolution tandem catalysts and investigate the adsorption and migration behaviors of *CO under interfacial electric fields. Electrochemical CO2 reduction test results indicate that the higher CO selectivity of Au/Cu is attributed to its weak *CO adsorption capacity, confirmed by in situ attenuated total reflection-infrared and in situ Raman. The low C2+ selectivity of Pd/Cu is owing to its high reaction energy barrier and low catalytic activity. In contrast, Ag/Cu achieves a high FEC2+ of 89.2% and a partial current density (jc2+) of 553.9 mA cm2 thanks to the low reaction energy barrier and moderate *CO adsorption capacity. COMSOL multiphysics simulations reveal that the effect of the interfacial electric field on *CO external migration could be neglected in the nanometer range. Although a strong interfacial electric field increases the energy barrier for internal migration of *CO, the enhanced adsorption capacity of *CO still dominates C–C coupling in the *CO-rich microenvironment over tandem catalysts.

DOI: 10.1002/anie.202511704

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202511704