Photocatalytic Oxidation of Methane to Methanol by Tungsten Trioxide-supported Atomic Gold at Room Temperature

TLDR: In this paper, an atomically dispersed gold on tungsten trioxide (Au1/WO3) catalyst for photocatalytic oxidation of methane toward value-added methanol was reported.

Abstract: Atomic-scale metals as active center have been widely investigated for efficient photocatalysis. Understanding the specific electronic structure of atomic-scale center is of frofound fundamental importance for superior catalytic performance. Here, we report an atomically dispersed gold on tungsten trioxide (Au1/WO3) catalyst for photocatalytic oxidation of methane toward value-added methanol. The Au1 species reveal a specific tip-enhanced local electrons field which favors the C-H dehydrogenation of methane and thus form methanol (up to 589 µmol g-1 h-1). Both experimental and theoretical results demonstrate such tip-enhanced effect-dependent activity of methane oxidation. The theoretical calculations further reveal a lower adsorption energy of product methanol on Au1, in contrast to Au particles, which suppresses the overoxidation of methanol, and thus promotes its selectivity. Establishing the electric structure-activity may create a platform for designing efficient atomic-scale catalysts for C1 catalysis and green chemistry.