Interfacial modulation promoted CC coupling in selective methane oxidation to ethanol

IF 4.4 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2026-09-01 DOI:10.1002/aic.70637

Ke‐Xin Li, Weimin Huang, Jingwen Huang, Zhenyuan He, Shanshan Chen, Shifeng Wang, Yong Li, Yuanhao Wang, Zhun Hu

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引用次数: 0

Abstract

Selective methane oxidation to ethanol remained a formidable challenge. Herein, MOF‐derived In 2 O 3 was synthesized via MIL‐68(In) pyrolysis. The optimized In 2 O 3 ‐500 achieved an ethanol yield of 10.8 mmol·g −1 ·h −1 under full‐spectrum illumination. These performances were attributed to carboxylate type CO related interfacial modulation, which enriched surface electron density and promoted CC coupling. During derivation, precursor derived carbon species were retained as carboxylate type CO related structures and interacted with the InO framework, inducing surface charge redistribution. Compared with In 2 O 3 ‐400, which retained residual MOF structures, and highly crystalline In 2 O 3 ‐600, which exhibited severe charge recombination, In 2 O 3 ‐500 exhibited a higher surface electron density and enhanced ·OH and ·CH 3 generation, thereby promoting the stepwise oxidation of *CH 3 to *CH 3 O and *CH 2 O. The enriched *CH 2 O and *CH 3 intermediates further facilitated C–C coupling to form ethanol. These findings highlighted the role of electron‐rich surfaces in steering methane conversion toward ethanol.

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界面调制促进了甲烷选择性氧化制乙醇过程中C - γ - C偶联

选择性甲烷氧化制乙醇仍然是一个艰巨的挑战。本文通过MIL - 68（In）热解合成了MOF衍生的in2o3。在全光谱照明下，优化后的in2o3‐500的乙醇产率为10.8 mmol·g−1·h−1。这些性能归因于羧酸型C - O相关的界面调制，它丰富了表面电子密度，促进了C - C耦合。在衍生过程中，前驱体衍生的碳种被保留为羧酸型C - O相关结构，并与In - O框架相互作用，诱导表面电荷重新分布。与保留剩余MOF结构的in2o3‐400和表现出严重电荷重组的in2o3‐600相比，in2o3‐500表现出更高的表面电子密度，并增强了·OH和·CH 3的生成，从而促进了*CH 3逐步氧化为*CH 3 O和*CH 2 O。富集的*CH 2 O和*CH 3中间体进一步促进了C-C偶联形成乙醇。这些发现强调了富电子表面在将甲烷转化为乙醇中的作用。

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.