数字农科院2.0

Selective photocatalytic oxidation of methane to formaldehyde based on ·OOH radical guidance over ZIF-8 Derived Au-ZnO

文献类型： 外文期刊

作者： Yi Xie;Yuhang Shao;Zitong Bao;Shengrong Zhou;Wenguo Wang;Liangwei Deng;Hongwei Zhang

作者机构：

关键词： formaldehyde selectivity;methane oxidation;photocatalysis;ZIF-8 derived Au-ZnO;·OOH radical guidance

期刊名称： Chemical Engineering Journal

ISSN： 1385-8947

年卷期： 2025 年 523 卷

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： Methane (CH4), serving as a critical energy source and a potent greenhouse gas, has drawn significant attention due to its potential for selective conversion into value-added chemicals such as formaldehyde (HCHO) and methanol (CH3OH). However, achieving partial oxidation of CH4 under mild conditions remains highly challenging due to its chemical inertness and tendency toward overoxidation. Herein, we report a ZIF-8-derived Au nanoparticle-loaded ZnO photocatalyst (Au-ZnO) via controlled pyrolysis, which enables efficient and highly selective CH4 oxidation to HCHO at ambient temperature (25 °C). The optimized 0.2Au-ZnO catalyst (0.19 wt% Au loading) exhibits exceptional performance, achieving an HCHO production rate of 8.65 mmol g−1 h−1 and a selectivity of 76.3 %, significantly outperforming counterparts modified with other noble metals (Pt, Ru, Pd, Ag). Mechanistic studies demonstrate that uniformly dispersed Au nanoparticles (~33 nm) promote interfacial electron separation efficiency while concurrently generating dual reactive oxygen species (·OOH and ·OH). In situ DRIFTS and EPR spectroscopy confirm that CH4 oxidation proceeds via an ·OOH-dominated pathway: photogenerated ·CH3 radicals preferentially couple with ·OOH to form transient CH3OOH intermediates, which rapidly dehydrate to yield HCHO, thereby suppressing the competing ·OH-driven route to methanol. This work establishes a novel ·OOH radical guided photocatalytic strategy for selective C[sbnd]H bond activation in CH4, advancing solar-driven CH4 valorization.

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