Efficient and Selective Photocatalytic Oxidation of CH<sub>4</sub> over Fe Single-Atom-Incorporated MOFs under Visible Light
Chengcheng Zhang, Yingkui Yan, Hubiao Huang, Xinsheng Peng, Hui Song, Jinhua Ye, Li Shi
Abstract
Photocatalytic CH 4 oxidation to liquid products under room temperature is a promising way for maximizing the value of CH 4 . However, the selective oxidation of CH 4 is a big challenge due to the high dissociation energy of CH 4 and the high reactivity of liquid products. Here, we report the Fe single-atom-incorporated metal–organic framework (Fe@PCN-222) as an effective and selective photocatalyst for photocatalytic oxidation of CH 4 to liquid oxygenates (CH 3 OH and HCHO) under visible light at room temperature. Fe@PCN-222 exhibits a liquid oxygenate yield of 19.0 μmol in 2 h and a selectivity of 88.4% in the presence of 400 μmol H 2 O 2 and 2 MPa CH 4, far exceeding that of the bare PCN-222 photocatalyst. The Fe single-atoms in PCN-222 not only promote the photogenerated electron transfer but also facilitate the activation of H 2 O 2 to produce active ·OH, which synergistically results in a substantial improvement of selectivity and activity of liquid oxygenate production.