Precise Regulation of Oxygen Vacancy in Cu/SiO 2 Catalysts Enhances Carbonyl Adsorption for Efficient Hydrogenation of Cyclic Carbonates

催化作用 吸附 氧气 空位缺陷 材料科学 无机化学 化学 化学工程 物理化学 有机化学 结晶学 工程类
作者
Xiumin Huang,Hangkong Yuan,Dongcheng He,Ce Liu,Xinjiang Cui,Feng Shi
出处
期刊:ChemistrySelect [Wiley]
卷期号:10 (30)
标识
DOI:10.1002/slct.202502836
摘要

Abstract The indirect conversion of carbon dioxide (CO 2 ) is one of the important pathways to reduce greenhouse effect and achieve CO 2 conversion and utilization. The reaction route from CO 2 with epoxy compounds to produce methanol and ethylene glycol via ethyl carbonate intermediate is attracted widespread attention due to the lower thermodynamic energy barrier and 100% elements utilization in CO 2 . However, the ethyl carbonate hydrogenation to methanol as the part of the route is still limited by excessive metal loading, high H 2 /ethylene carbonate (EC) molar ratios, and insufficient stability. In this study, copper (Cu)‐based catalyst containing surface oxygen vacancy is developed via the sol–gel (SG) method to promote hydrogenation of ethyl carbonate, based on the adsorption of carbonyl groups by oxygen vacancy (O v ). Noted that the optimal catalyst of 8Cu/SiO 2 ‐SG exhibits excellent catalytic performance (99% conversion of ethyl carbonate, 99% yield of ethylene glycol and 96% yields methanol) under moderate conditions and operate stably over 120 h in stability testing. The experimental and characterization results show that the concentration of O v in catalyst is positively correlated with the methanol yield, which suggest that the precise regulation of O v enhances carbonyl adsorption and improve the catalytic performance. This work provides a rational design strategy for efficient hydrogenation catalysts.
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