Angew. Chem. Paper on Tailoring Hydrogenation Pathway for Selective Ethanol Conversion Published! Congrats to Zihong!

Electrochemical CO2 reduction to ethanol faces a fundamental challenge: competing ethylene formation through shared C2 intermediates. While previous studies focused on modifying catalyst electronic structures or increasing *CO coverage, the critical role of competitive hydrogenation pathways remains unexplored. Here, we demonstrate that the selectivity between ethanol and ethylene is governed by the balance between Langmuir–Hinshelwood (surface *H) and Eley–Rideal (solvent H) hydrogenation mechanisms. Through hierarchically assembled BPEI/PT interfaces, we dynamically modulate this balance by reconstructing

interfacial hydrogen-bond networks without altering catalyst electronic properties.In situ Raman spectroscopy captures enhanced *OCHCH2/*OCHCH3 intermediates, directly correlating ethanol selectivity with suppressed ER pathway. Combined experimental and theoreti calstudies establish quantitative relationships between hydrogen-bond strength and pathway selectivity. This strategy achieves 38.7% ethanol Faradaic efficiency (FE) at 900 mA cm−2 on CuO-derived catalysts (116% improvement) and 53% at 800 mA cm−2 on CuAg systems—among the highest reported efficiencies. Our findings reveal that controlling competitive hydrogenation pathways through interfacial engineering provides an independent parameter for steering CO2 reduction selectivity.

论文链接

https://onlinelibrary.wiley.com/doi/10.1002/anie.202523475