Modulating Chloride Adsorption for Efficient Chloride-Mediated Methane Conversion over Tungsten Oxide Photoanode

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-03-30 DOI:10.1021/acscatal.4c07046

Jun Ma, Keke Mao, Jiayi Li, Guangyao Zhai, Di Wu, Dong Liu, Ran Long, Yujie Xiong

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Abstract

Utilizing alkali chlorides as the chloride source in chloride-mediated methane activation represents an efficient approach for CH₄ valorization. Nevertheless, great challenges remain due to the restricted catalytic activity and durability. Here, we present a photoelectrochemical approach for chloride-mediated methane conversion to C₁ products using WO₃ with surface oxygen vacancies (OV). Theoretical calculations indicate that oxygen vacancies play a crucial role in enhancing chloride adsorption to facilitate methane activation. The engineered WO₃–OV photoanode exhibits enhanced catalytic performance in comparison to the pristine counterparts, attaining a Faradaic efficiency of 94.5% for C₁ products (methyl chloride, methanol, formic acid, and formaldehyde) at 0.9 V vs RHE. This performance corresponds to a total production rate of 139.2 mmol g^–1 h^–1 for the C₁ products. Furthermore, the system is capable of achieving a high CH₄ conversion efficiency of 11.8%. This work emphasizes the pivotal role of photoanode design and surface engineering in facilitating methane conversion.

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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.