Highly Selective Photocatalytic Methane Oxidation to Methanol Using CO<sub>2</sub> as a Soft Oxidant
Yongping Gan, Min Huang, Fei Yu, Yu Xing, Zhanjun He, Jin Liu, Tiejun Lin, Yuanyuan Dai, Qiang Niu, Liangshu Zhong
Abstract
Light-driven methane conversion to methanol with high selectivity is considered a challenging and promising reaction for sustainable development. Herein, Cu/CeO 2 catalysts were prepared for photocatalytic methane conversion with CO 2 as a soft oxidant. Methanol was the sole liquid product with a high selectivity of 96.2% and a high yield of 88.9 μmol g –1 h –1 for the 2Cu/CeO 2 catalyst. Investigation of the structure–performance relationship indicated that oxygen vacancies facilitated the trapping of photogenerated electrons and avoided carrier recombination. In addition, as a soft oxidant, CO 2 can also capture photogenerated electrons to be reduced to CO and further accelerate the formation of CH 3 OH. A catalytic mechanism study demonstrated that methane and hydroxyl were oxidized by photogenerated holes to • CH 3 and • OH, respectively, and thus, methanol was generated through the combination of • CH 3 and • OH.