W Single‐Atom Catalyst for CH<sub>4</sub> Photooxidation in Water Vapor
Ye Wang, Jiangwei Zhang, Wenxiong Shi, Gui‐Lin Zhuang, Qiu‐Ping Zhao, Jing Ren, Peng Zhang, Hua‐Qing Yin, Tong‐Bu Lu, Zhiming Zhang
Abstract
Abstract Solar‐driven high‐efficiency and direct conversion of methane into high‐value‐added liquid oxygenates against overoxidation remains a great challenge. Herein, facile and mass fabrication of low‐cost tungsten single‐atom photocatalysts is achieved by directly calcining urea and sodium tungstate under atmosphere (W‐SA‐PCN‐ m , urea amount m = 7.5, 15, 30, and 150 g). The single‐atom photocatalysts can manage H 2 O 2 in situ generation and decomposition into ·OH, thus achieving highly efficient CH 4 photooxidation in water vapor under mild conditions. Systematic investigations demonstrate that integration of multifunctions of methane activation, H 2 O 2 generation, and decomposition into one photocatalyst can dramatically promote methane conversion to C1 oxygenates with a yield as high as 4956 µmol g cat −1 , superior to that of the most reported non‐precious photocatalysts. Liquid–solid phase transition can induce the products to facilely switch in from HCOOH to CH 3 OH by pulling the catalyst above water with CH 3 OH/HCOOH ratio from 10% (in H 2 O) to 80% (above H 2 O).