乙炔
乙烯
氢
催化作用
材料科学
光化学
法拉第效率
聚合物
电催化剂
可逆氢电极
X射线光电子能谱
密度泛函理论
电极
化学
氢气储存
工作(物理)
化学工程
膜
乙二醇
无机化学
电流密度
作者
Lei Bai,Xiao Han,Dingding Li,Chuncai Kong,Jingbo Shi,Mengyao She,Jian Bai,Jinbo Bai,Kunyue Leng,Yafei Zhao,Yue Lin,L S Zheng,YunTeng Qu
标识
DOI:10.1038/s41467-025-67764-8
摘要
Electroconversion of acetylene towards polymer-grade ethylene (EAE) is recognized as a promising substitution for thermo-catalytic route. The excessive active-hydrogen supplies a high current density induces the conspicuous hydrogen evolution, reducing the ethylene Faradaic efficiency (FE). Here, we develop a Cu-Pd single atom alloy (SAA) catalyst, achieving a 90.5% FE with a large ethylene partial current density of -1.16 A cm-2, and maintain stability for 110 h at -0.2 A cm-2 in the flow-cell system. In membrane electrode assembly, Cu-Pd SAA delivers a 90.1% ethylene FE and ~100 % conversion at -2.5 A (-0.1 A cm-2), along with 500 h stability for crude ethylene purification. Combined in-situ spectroscopy and DFT calculation reveal that the catalyst facilitates the direct hydrogenation of acetylene via Pd-H species rather than hydrogen spillover. This mechanism concurrently lowers the EAE energy barrier and suppresses the hydrogen evolution reaction. This work provides insights for designing high-efficiency electrocatalysts for hydrogenation electrosynthesis.
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