美国宾夕法尼亚大学Anthony Shoji Hall团队揭示了无序界面H₂O促进电化学C-C耦合。这一研究成果发表在2025年7月23日出版的《自然-化学》杂志上。

人们对将二氧化碳和一氧化碳转化为能量密集的多碳产品以帮助缓解气候变化的兴趣越来越大，但由于竞争途径的存在，引导选择性仍然具有挑战性。

研究组表明，调整以高浓度氯化钠电解质为主体的界面水结构，可以促进CO电还原为C₂H₄。将 NaClO₄浓度从 0.01 molal 提升至 10 molal 后，CO 还原反应速率提升 18 倍，在相对于标准氢电极（NHE）仅需 -1.43 V 电压条件下，多碳产物的法拉第效率达 91%。温度依赖性CO还原，结合表面增强拉曼光谱，揭示了界面H₂O结构的变化对应于CO还原为C₂H₄的表观活化焓和熵的变化。在较高的离子强度下，激活熵的增加与氢键的破坏和非氢键水模式的出现有关，这表明无序的界面H₂O层有助于CO还原为C₂H₄。这些发现为如何控制界面水的结构来促进CO还原成多碳产物提供了有价值的见解。

附：英文原文

Title: Disordered interfacial H2O promotes electrochemical C–C coupling

Author: Zhang, Hao, Raciti, David, Hall, Anthony Shoji

Issue&Volume: 2025-07-23

Abstract: There is growing interest in the conversion of CO2 and CO into energy-dense multi-carbon products to help mitigate climate change, but guiding selectivity remains challenging due to competing pathways. Here we show that tuning the structure of interfacial water using highly concentrated NaClO4 electrolytes enhances CO electroreduction to C2H4. Increasing the NaClO4 concentration from 0.01 to 10molal increased the CO reduction rate 18-fold, achieving a Faradaic efficiency of 91% for multi-carbon products at 1.43V versus the normal hydrogen electrode. Temperature-dependent CO reduction, combined with surface-enhanced Raman spectroscopy, revealed that changes in the interfacial H2O structure correspond to variations in the apparent activation enthalpy and entropy for the reduction of CO to C2H4. At higher ionic strength, increases in activation entropy were linked to disrupted hydrogen bonding and the emergence of non-hydrogen-bonded water modes, suggesting that disordered interfacial H2O layers facilitate CO reduction to C2H4. These findings offer valuable insights into how manipulating the structure of interfacial water can enhance the reduction of CO to multi-carbon products.

DOI: 10.1038/s41557-025-01859-z

Source: https://www.nature.com/articles/s41557-025-01859-z