数字农科院2.0

Direct oxidation of trace methane to formaldehyde under ambient conditions by piezo-photocatalytic synergy

文献类型： 外文期刊

作者： Qiyu Zhang;Li Rong;Yue Jiang;Zhiping Zhu;Xiaochang Lin;Yongzhen Ding;Hongmin Dong;Dezhao Liu

作者机构：

关键词： Efficient carrier separation;Piezo-photocatalysis;Piezoelectric effect;Trance methane conversion

期刊名称： Chemical Engineering Journal

ISSN： 1385-8947

年卷期： 2025 年 524 卷

页码：

收录情况： SCIE（2025版） ; ; EI（2025版）

摘要： Methane conversion under ambient conditions has garnered significant attention due to complex catalyst design, costly oxidants, and unwanted byproducts remain. In this study, we established a newly discovered process for the direct conversion of methane under ambient conditions by leveraging the concept of piezo-photocatalysis, which synergistically integrates energy input from both light irradiation and ultrasonic vibration. An efficient formaldehyde (HCHO) yield of 11.07 μmol·g−1·h−1 was achieved by using the piezo-photocatalyst system BaTiO3/g-C3N4 (2BTO/CN), which is approximately 3.5 times higher than that under ultrasonic vibration alone (3.2 μmol·g−1·h−1) and 2.6 times higher than that under simulated solar irradiation alone (4.27 μmol·g−1·h−1). Under optimal conditions, the yield can reach a maximum of 60.79 μmol·g−1·h−1. The enhanced performance is attributed to the ultrasonic vibration-induced generation of polarized electric fields within g-C3N4 which sustain the built-in electric field intensity at the heterojunction interface. This facilitates more efficient migration of photogenerated charge carriers, improving charge separation efficiency and enabling the synergistic catalytic effect of piezoelectricity under simulated solar irradiation. Electron paramagnetic resonance (EPR) spectroscopy revealed enhanced signals from hydroxyl radicals (·OH) and superoxide radicals (·O2−) under synergistic conditions. Additionally, density functional theory (DFT) calculations demonstrated that, under ultrasound-assisted conditions, the energy barrier for the rate-determining step of methane photocatalytic conversion on BaTiO3/g-C3N4 is significantly reduced. The implications of this methodology, with its potential for broader application in gas-phase catalytic reactions, underscore a significant advance in catalysis.

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