近日，浙江大学侯阳团队报道了分子工程化共价疏水界面用于强酸中增强二氧化碳电甲烷化。2026年2月24日，《国家科学评论》杂志发表了这一成果。

将二氧化碳电化学转化为甲烷为燃料合成提供了一条可持续途径，但该方法本质上难以平衡碳利用效率与产物选择性之间的矛盾。基于物理疏水涂层的传统表面工程策略常导致界面不稳定和电荷传输效率下降。

针对这些问题，研究组开发了一种半胱氨酸包覆的铜配位络合物催化剂，通过共价键合氟烷基硅烷（FAS）实现表面润湿性的精确调控。研究在强酸性电解液中取得突破，在400 mA cm^-2电流密度（pH 1.8）条件下，甲烷法拉第效率高达66.2%，单程碳转化效率达31.1%，超越了传统碱性体系的性能基准。

表面增强拉曼光谱揭示了CO₂活化的关键COOH中间体，原位ATR-FTIR光谱则追踪了通过CHO和*CH₂O中间体的逐步氢化反应路径。分子动力学模拟进一步揭示，FAS涂层诱导的疏水共价界面在催化剂表面附近形成了独特的水分子排除区。这种界面工程策略通过阻隔水分子接触抑制析氢反应，在反应过程中保持疏水性，为提升CO₂电还原反应动力学和选择性提供了可规模化的发展路径。

附：英文原文

Title: Molecularly engineered covalent hydrophobic interface for enhanced CO2 electromethanation in strong acid

Author: Zhu, Chang, Wang, Dashuai, Liu, Nengji, Lin, Weixiao, Zeng, Libin, Chen, Yaqi, Zheng, Wanzhen, Peng, Xianyun, Feng, Guanghui, Li, Zhongjian, Yang, Bin, Sang, Xiahan, Lei, Lecheng, Song, Fei, Samorì, Paolo, Hou, Yang

Issue&Volume: 2026-02-24

Abstract: Electrochemical conversion of CO2 to methane provides a sustainable pathway for fuel synthesis, yet it inherently struggles to balance carbon utilization efficiency with product selectivity. Conventional surface engineering based on physical hydrophobic coatings often leads to interfacial instability and diminished charge transfer efficiency. To address these issues, we develop a cysteine-coated copper coordination complex catalyst modified with covalently bonded fluoroalkyl silane (FAS), allowing precise control over surface wettability. A breakthrough in highly acidic electrolytes is demonstrated, achieving a methane Faradaic efficiency of up to 66.2% at 400 mA cm2 (pH 1.8), alongside a single-pass carbon conversion efficiency of 31.1%, surpassing conventional alkaline-system benchmarks. Surface-enhanced Raman spectroscopy reveals key *COOH intermediate for CO2 activation, while in situ ATR-FTIR spectroscopy monitors the sequential hydrogenation pathway through *CHO and *CH2O. Molecular dynamics simulations further reveal a distinct water exclusion zone near the catalyst surface, which arises from the hydrophobic covalent interface induced by the FAS coating. This interfacial engineering strategy suppresses the hydrogen evolution reaction by blocking water access, preserves hydrophobicity during operation, and offers a scalable path to improve the kinetics and selectivity of CO2 electroreduction.

DOI: 10.1093/nsr/nwag116

Source: https://dx.doi.org/10.1093/nsr/nwag116