A tandem electro-thermocatalysis platform for practical hydrogen peroxide-mediated oxygenation reactions at high rates

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2025-06-11 DOI:10.1002/aic.18930

Huijie Chen, Menglu Cai, Jianbo Shao, Ting Lin, Yan Liu, Yiming Mo

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Abstract

Hydrogen peroxide (H₂O₂) is a platform green oxidant for high-value chemical synthesis, but its centralized production hinders its widespread use in a safe manner. Here, we describe a practical tandem electro-thermochemical H₂O₂-mediated oxygenation platform for the synthesis of various high-value oxygen-containing compounds. The integration of solid-electrolyte H₂O₂ electrosynthesis with heterogeneous zeolite thermocatalysis enables atom-efficient oxygenations without the need for downstream electrolytes or catalysts separation. A spatially decoupled tandem system integrating aqueous H₂O₂ electrosynthesis with nonaqueous thermocatalysis offers independent optimization capabilities, thus maximizing the overall space–time yield (STY). With microfluidic packed-bed intensification for heterogeneous thermocatalysis, this tandem system achieved H₂O₂-mediated oxygenation of thioesters to sulfoxide at a high current density (300 mA cm⁻²) and STY (7.07 mmol cm⁻³ h⁻¹). Furthermore, the platform's broad applicability was showcased with titanium-silicalite-1 zeolite catalyzed olefin epoxidation and cyclohexanone oxime synthesis, underscoring its potential for diverse catalytic oxygenation applications.

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串联电-热催化平台，用于实际过氧化氢介导的高速率氧化反应

过氧化氢（H2O2）是高价值化工合成的平台型绿色氧化剂，但其集中生产阻碍了其安全广泛应用。在这里，我们描述了一个实用的串联电-热化学h2o2介导的氧化平台，用于合成各种高值含氧化合物。固体电解质H2O2电合成与非均相沸石热催化相结合，无需下游电解质或催化剂分离，即可实现原子高效氧合。将水相H2O2电合成与非水相热催化相结合的空间解耦串联系统提供了独立的优化能力，从而最大化了整体时空产率（STY）。采用微流控填料床强化非均相热催化技术，该串联系统在高电流密度（300 mA cm - 2）和高速度（7.07 mmol cm - 3 h - 1）下实现了硫酯在h2o2介导下氧化生成亚砜。此外，该平台的广泛适用性在钛-硅-1沸石催化烯烃环氧化和环己酮肟合成中得到了展示，强调了其在多种催化氧化应用中的潜力。

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

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.