A spatially integrated electrochemical–thermal tandem reaction for continuous mild synthesis of propylene oxide†

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-10-02 DOI:10.1039/D4GC03455D

Yuefeng Qiu, Peng Jiang, Wenkai Ye, Jiahao Hu, Bin Zhang, Tuo Ji, Liwen Mu, Xin Feng, Xiaohua Lu and Jiahua Zhu

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Abstract

An electrochemical–thermal tandem reaction system was designed in this work and enabled the highly efficient synthesis of propylene oxide (PO) at 1 atm without the use of H₂O₂. The electrochemical part produced OOH⁻ through a 2e⁻ oxygen reduction reaction, which migrated and distributed in the full space of a chamber filled with a mixture of solid electrolyte particles and modified TS-1 (m-TS-1) catalysts. Mediated by the relay of OOH⁻ and protic solvent methanol, full space tandem reactions were achieved with a high PO selectivity of 95.2% and a productivity of 319.75 mmol g_ecat⁻¹ h⁻¹. A mechanistic study revealed that the m-TS-1 catalysts accepted the migrated OOH⁻ and formed a Ti-OOH intermediate, which played a key role in relaying the tandem reactions for an efficient propylene epoxidation reaction. Techno-economic analysis and life-cycle assessment revealed favorable figures for the proposed process compared to the conventional process.

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用于环氧丙烷连续温和合成的空间集成电化学-热串联反应

这项工作设计了一个电化学-热串联反应系统，该系统能够在 1 atm 下高效合成环氧丙烷 (PO)，而无需使用 H2O2。电化学部分通过 2e- 氧还原反应产生 OOH-，OOH- 在充满固体电解质颗粒和改性 TS-1 （m-TS-1）催化剂混合物的腔室的整个空间中迁移和分布。在 OOH- 和原生溶剂甲醇的中继作用下，实现了全空间串联反应，PO 选择性高达 95.2%，生产率为 319.75 mmol gecat-1 h-1。机理研究表明，m-TS-1 催化剂接受了迁移的 OOH- 并形成了 Ti-OOH 中间体，该中间体在高效丙烯环氧化反应的串联反应中发挥了关键作用。技术经济分析和生命周期评估显示，与传统工艺相比，拟议工艺的数据更为有利。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.