Propylene Epoxidation using Molecular Oxygen over Copper- and Silver-Based Catalysts: A Review,ACS Catalysis

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Propylene Epoxidation using Molecular Oxygen over Copper- and Silver-Based Catalysts: A Review
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-11-03 , DOI: 10.1021/acscatal.0c03340
Janvit Teržan _{1,

2} , Matej Huš ₁ , Blaž Likozar ₁ , Petar Djinović _{1,

3}

Affiliation

Propylene oxide (PO) is a versatile chemical, mainly used in the synthesis of polyurethane plastics. Propylene epoxidation using molecular oxygen could replace the tedious current synthesis protocols, which use expensive H₂O₂ or organic peroxides as oxidants. This review focuses on the propylene epoxidation reaction using molecular oxygen in the gas phase over copper- and silver-based catalysts. Silver is a proven and industrially used ethylene epoxidation catalyst. However, it initiates allylic hydrogen stripping (AHS) in propylene epoxidation, shifting the selectivity toward unwanted acrolein and total oxidation. Nevertheless, silver has been extensively studied to determine if AHS could be mitigated by targeted active site design and various doping strategies. Copper-based catalysts have been less extensively studied but have been experimentally proved as well as theoretically confirmed that their PO selectivity is on par with that of silver. In this review, different catalyst modification strategies have been analyzed and the achieved improvements discussed. Theoretical approaches aimed at understanding the mechanism and predicting catalytic performance on the basis of electronic states (density functional theory calculations) are also reviewed. We conclude with a future outlook on how the current state of the art knowledge of active site modification and reaction engineering approaches could leverage the PO selectivity toward industrial requirements, thus enabling a breakthrough in gas-phase propylene epoxidation using O₂.

中文翻译：

铜和银基催化剂上使用分子氧的丙烯环氧化研究进展

环氧丙烷（PO）是一种通用化学品，主要用于合成聚氨酯塑料。使用分子氧进行丙烯环氧化可以取代繁琐的电流合成规程，后者使用昂贵的H ₂ O ₂或有机过氧化物作为氧化剂。这篇综述的重点是在铜和银基催化剂上使用气相中的分子氧进行丙烯环氧化反应。银是一种行之有效的工业上使用的乙烯环氧化催化剂。但是，它会在丙烯环氧化反应中引发烯丙基氢汽提（AHS），从而将选择性转向不想要的丙烯醛和全部氧化反应。然而，已经对银进行了广泛的研究，以确定是否可以通过针对性的活性位点设计和各种掺杂策略来缓解AHS。铜基催化剂的研究较少，但已通过实验证明并在理论上证实它们的PO选择性与银相同。在这篇综述中，分析了不同的催化剂改性策略并讨论了所取得的改进。还综述了旨在了解机理并基于电子态预测催化性能的理论方法（密度泛函理论计算）。我们以对活性位点修饰和反应工程方法的最新知识如何利用PO选择性满足工业要求的方法得出未来展望，从而实现了使用O进行气相丙烯环氧化的突破₂。

更新日期：2020-11-21

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