posted on 2023-11-13, 13:12authored byChengcheng Zhang, Yingkui Yan, Hubiao Huang, Xinsheng Peng, Hui Song, Jinhua Ye, Li Shi
Photocatalytic
CH4 oxidation to liquid products under
room temperature is a promising way for maximizing the value of CH4. However, the selective oxidation of CH4 is a
big challenge due to the high dissociation energy of CH4 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 CH4 to liquid oxygenates (CH3OH 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 H2O2 and 2
MPa CH4, 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 H2O2 to produce active ·OH, which synergistically results
in a substantial improvement of selectivity and activity of liquid
oxygenate production.