催化作用
环氧丙烷
化学
选择性
密度泛函理论
单层
吸附
反应机理
光化学
活化能
分子轨道
物理化学
计算化学
分子
有机化学
生物化学
环氧乙烷
共聚物
聚合物
作者
Akanksha Ashok Sangolkar,Ravinder Pawar
标识
DOI:10.1002/cphc.202200334
摘要
Abstract The aerobic oxidation of propylene to selectively achieve propylene oxide (PO) is a challenging reaction in catalysis. Therefore, an active catalyst which shows enhanced PO selectivity is extremely desired. In the present investigation, an attempt has been made to explore the catalytic activity of a mono‐atomically thin two‐dimensional (2D) hexagonal (HX) Cu layer for selective propylene epoxidation using molecular O 2 with the aid of density functional theory calculations. The results reveal that the conversion of propylene to PO via Eley‐Rideal mechanism is an exoergic and barrierless reaction on the O 2 pre‐adsorbed Cu monolayer. The Pauli energy component plays a decisive role for barrierless reaction whereas the electrostatic and orbital contribution governs the energetic stability of PO. Car‐Parrinello molecular dynamics (CPMD) simulation reinforces the outcomes of climbing image nudged elastic band (CI‐NEB) calculation. Further, the formation of oxametallacycle OMC‐2 (0.47 eV) is kinetically favourable over OMC‐1 (0.87 eV) and AHS (0.50 eV) on O pre‐adsorbed 2D HX Cu. Interestingly, the energy barrier for the conversion of OMC‐2 to PO (0.70 eV) is considerably low in comparison with the acetone formation (0.90 eV). Therefore, it is worth to mention that the 2D HX Cu surface provides a promising platform for selective propylene epoxidation.
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