近日，中国科学院化学研究所刘志敏团队报道了在碳酸氢盐电解质中控制界面氢原子转移以电催化CO₂还原为乙烯。相关论文发表在2025年11月12日出版的《科学通报》杂志上。

铜基催化剂一直以来都被视为将CO₂转化为多碳产物（C₂₊产物）的潜力候选。然而，要实现针对特定C₂₊产物的选择性仍面临挑战，这需要通过对催化位点进行精细设计来调控反应路径的能量偏好。研究组通过在铜表面引入可产生活性氢原子（H）的催化位点，调控电催化CO₂加氢路径，实现了乙烯的选择性生成。

研究组通过理论计算从17种元素的51种结构中筛选出钌单原子位点（Ru₁），其展现出促进CO₂还原中间体加氢的最佳活性。据此合成的钌单原子掺杂氧化物衍生铜催化剂在KHCO₃电解液中，于C₂₊产物中实现82%的乙烯选择性，法拉第效率达58.9%，偏电流密度为353.4 mA cm^-2。动力学同位素与原位光谱分析证实，Ru₁位点通过调控H向中间体的转移，有效促进中间体加氢过程，从而推动形成能量最优的乙烯生成路径。这些研究结果为设计具有中间体加氢位点的铜催化剂以实现CO₂向特定产物的转化提供了新视角。

附：英文原文

Title: Manipulating interfacial hydrogen atom transfer for electrocatalytic CO2 reduction to ethylene in bicarbonate electrolyte

Author: Jiaju Fu a, Zhimin Liu a b

Issue&Volume: 2025/11/12

Abstract: Cu-based catalysts have been considered promising electrocatalysts for converting CO2 into multi-carbon products (C2+ products). However, achieving selectivity toward a specific C2+ product remains challenging, necessitating the delicate design of catalytic sites to regulate the energy preference of reaction pathways. Herein, we introduced catalytic sites that evolve active hydrogen atoms (*H) on Cu surfaces to regulate electrocatalytic CO2 hydrogenation pathways to achieve the selective production of ethylene. Ru single-atom site (Ru1) was theoretically screened from 17 elements with 51 structures, exhibiting optimal activity in promoting hydrogenation of CO2 reduction intermediates. The accordingly synthesized Ru1-doped oxide-derived Cu (Ru1-ODCu) catalyst delivered an ethylene selectivity of 82% in C2+ products with a Faradaic efficiency of 58.9% and a partial current density of 353.4 mA cm–2 in KHCO3 electrolyte. Kinetic isotope and in situ spectroscopic analyses evidenced that the Ru1 sites effectively promote intermediate hydrogenation by regulating *H transfer to intermediates, facilitating the energy-preferred pathway to ethylene production. These results provide insights into the design of Cu catalysts with intermediate hydrogenation sites for converting CO2 into specific products.

DOI: 10.1016/j.scib.2025.11.022

Source: https://www.sciencedirect.com/science/article/abs/pii/S2095927325011508