Light-driven flow synthesis of acetic acid from methane with chemical looping

Wenqing Zhang, Dawei Xi, Yihong Chen, Aobo Chen, Yawen Jiang, Hengjie Liu, Zeyu Zhou, Hui Zhang, Zhi Liu, Ran Long () and Yujie Xiong ()
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Wenqing Zhang: University of Science and Technology of China
Dawei Xi: University of Science and Technology of China
Yihong Chen: University of Science and Technology of China
Aobo Chen: University of Science and Technology of China
Yawen Jiang: University of Science and Technology of China
Hengjie Liu: University of Science and Technology of China
Zeyu Zhou: ShanghaiTech University
Hui Zhang: ShanghaiTech University
Zhi Liu: ShanghaiTech University
Ran Long: University of Science and Technology of China
Yujie Xiong: University of Science and Technology of China

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Oxidative carbonylation of methane is an appealing approach to the synthesis of acetic acid but is limited by the demand for additional reagents. Here, we report a direct synthesis of CH3COOH solely from CH4 via photochemical conversion without additional reagents. This is made possible through the construction of the PdO/Pd–WO3 heterointerface nanocomposite containing active sites for CH4 activation and C–C coupling. In situ characterizations reveal that CH4 is dissociated into methyl groups on Pd sites while oxygen from PdO is the responsible for carbonyl formation. The cascade reaction between the methyl and carbonyl groups generates an acetyl precursor which is subsequently converted to CH3COOH. Remarkably, a production rate of 1.5 mmol gPd–1 h–1 and selectivity of 91.6% toward CH3COOH is achieved in a photochemical flow reactor. This work provides insights into intermediate control via material design, and opens an avenue to conversion of CH4 to oxygenates.

Date: 2023
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DOI: 10.1038/s41467-023-38731-y

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