Molecular oxygen enhances H2O2 utilization for the photocatalytic conversion of methane to liquid-phase oxygenates

Xiao Sun, Xuanye Chen, Cong Fu, Qingbo Yu, Xu-Sheng Zheng, Fei Fang, Yuanxu Liu, Junfa Zhu, Wenhua Zhang and Weixin Huang ()
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Xiao Sun: University of Science and Technology of China
Xuanye Chen: University of Science and Technology of China
Cong Fu: University of Science and Technology of China
Qingbo Yu: Anhui University of Science and Technology
Xu-Sheng Zheng: University of Science and Technology of China
Fei Fang: University of Science and Technology of China
Yuanxu Liu: Anhui University of Chinese Medicine, Anhui Academy of Chinese Medicine
Junfa Zhu: University of Science and Technology of China
Wenhua Zhang: University of Science and Technology of China
Weixin Huang: University of Science and Technology of China

Nature Communications, 2022, vol. 13, issue 1, 1-12

Abstract: Abstract H2O2 is widely used as an oxidant for photocatalytic methane conversion to value-added chemicals over oxide-based photocatalysts under mild conditions, but suffers from low utilization efficiencies. Herein, we report that O2 is an efficient molecular additive to enhance the utilization efficiency of H2O2 by suppressing H2O2 adsorption on oxides and consequent photogenerated holes-mediated H2O2 dissociation into O2. In photocatalytic methane conversion over an anatase TiO2 nanocrystals predominantly enclosed by the {001} facets (denoted as TiO2{001})-C3N4 composite photocatalyst at room temperature and ambient pressure, O2 additive significantly enhances the utilization efficiency of H2O2 up to 93.3%, giving formic acid and liquid-phase oxygenates selectivities respectively of 69.8% and 97% and a formic acid yield of 486 μmolHCOOH·gcatalyst−1·h−1. Efficient charge separation within TiO2{001}-C3N4 heterojunctions, photogenerated holes-mediated activation of CH4 into ·CH3 radicals on TiO2{001} and photogenerated electrons-mediated activation of H2O2 into ·OOH radicals on C3N4, and preferential dissociative adsorption of methanol on TiO2{001} are responsible for the active and selective photocatalytic conversion of methane to formic acid over TiO2{001}-C3N4 composite photocatalyst.

Date: 2022
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DOI: 10.1038/s41467-022-34563-4

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