Regulating Au coverage for the direct oxidation of methane to methanol
Yueshan Xu, Daoxiong Wu, Qinghua Zhang, Peng Rao, Peilin Deng, Mangen Tang, Jing Li, Yingjie Hua, Chongtai Wang, Shengkui Zhong, Chunman Jia, Zhongxin Liu, Yijun Shen, Lin Gu, Xinlong Tian, Quanbing Liu
Abstract
Abstract The direct oxidation of methane to methanol under mild conditions is challenging owing to its inadequate activity and low selectivity. A key objective is improving the selective oxidation of the first carbon-hydrogen bond of methane, while inhibiting the oxidation of the remaining carbon-hydrogen bonds to ensure high yield and selectivity of methanol. Here we design ultrathin Pd x Au y nanosheets and revealed a volcano-type relationship between the binding strength of hydroxyl radical on the catalyst surface and catalytic performance using experimental and density functional theory results. Our investigations indicate a trade-off relationship between the reaction-triggering and reaction-conversion steps in the reaction process. The optimized Pd 3 Au 1 nanosheets exhibits a methanol production rate of 147.8 millimoles per gram of Pd per hour, with a selectivity of 98% at 70 °C, representing one of the most efficient catalysts for the direct oxidation of methane to methanol.