环氧丙烷
过氧化氢
催化作用
脱氢
化学
电解质
选择性
氧气
无机化学
化学工程
有机化学
物理化学
环氧乙烷
聚合物
激进的
工程类
电极
共聚物
作者
Hao Li,Christina Susan Abraham,Megha Anand,Ang Cao,Jens K. Nørskov
标识
DOI:10.1021/acs.jpclett.2c00257
摘要
Propylene oxide (PO) is an important chemical. So far, its synthesis protocol relies on expensive oxidants. In contrast, direct epoxidation of propylene (DEP) using molecular oxygen is considered ideal for PO synthesis. Unfortunately, DEP has not met industrial demands due to the low propylene conversion and high side-product selectivity for known catalysts. Instead of a thermal process using molecular oxygen, electrolytic propylene oxidation can synthesize PO at room temperature, using the atomic oxygen generated from water-splitting. Herein, using density functional theory, surface Pourbaix analysis, scaling relation analysis, and microkinetic modeling, we show that (i) propylene epoxidation is facile on weak-binding catalysts if reactive atomic oxygen preexists; (ii) electrolytic epoxidation is facile to provide atomic oxygen for epoxidation, while hydroperoxyl formation does not overwhelm the epoxidation process at the potential of interest; (iii) propylene dehydrogenation is a competing step that forms side products. Finally, we discuss the opportunities and challenges of this green PO synthesis method.
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