乙炔
乙烯
材料科学
催化作用
电化学
氢
光化学
选择性
无机化学
化学工程
电极
有机化学
化学
物理化学
工程类
作者
Zeping Wang,Lu Shang,Hongzhou Yang,Yunxuan Zhao,Geoffrey I. N. Waterhouse,Dong Li,Run Shi,Tierui Zhang
标识
DOI:10.1002/adma.202303818
摘要
Electrochemical acetylene reduction (EAR) is a promising strategy for removing acetylene from ethylene-rich gas streams. However, suppressing the undesirable hydrogen evolution is vital for practical applications in acetylene-insufficient conditions. Herein, Cu single atoms are immobilized on anatase TiO2 nanoplates (Cu-SA/TiO2 ) for electrochemical acetylene reduction, achieving an ethylene selectivity of ≈97% with a 5 vol% acetylene gas feed (Ar balance). At the optimal Cu-single-atom loading, Cu-SA/TiO2 is able to effectively suppress HER and ethylene over-hydrogenation even when using dilute acetylene (0.5 vol%) or ethylene-rich gas feeds, delivering a 99.8% acetylene conversion, providing a turnover frequency of 8.9 × 10-2 s-1 , which is superior to other EAR catalysts reported to date. Theoretical calculations show that the Cu single atoms and the TiO2 support acted cooperatively to promote charge transfer to adsorbed acetylene molecules, whilst also inhibiting hydrogen generation in alkali environments, thus allowing selective ethylene production with negligible hydrogen evolution at low acetylene concentrations.
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