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

doi:10.1038/s41467-024-44839-6

Regulating Au coverage for the direct oxidation of methane to methanol

Nat Commun. 2024 Jan 17;15(1):564. doi: 10.1038/s41467-024-44839-6.

Authors

Yueshan Xu^#¹, Daoxiong Wu^#¹, Qinghua Zhang^#², Peng Rao¹, Peilin Deng³, Mangen Tang¹, Jing Li¹, Yingjie Hua⁴, Chongtai Wang⁴, Shengkui Zhong⁵, Chunman Jia¹, Zhongxin Liu¹, Yijun Shen¹, Lin Gu^{6

7}, Xinlong Tian⁸, Quanbing Liu⁹

Affiliations

¹ School of Marine Science and Engineering, Hainan Provincial Key Lab of Fine Chemistry, School of Chemistry and Chemical Engineering, Hainan University, Haikou, 570228, China.
² Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
³ School of Marine Science and Engineering, Hainan Provincial Key Lab of Fine Chemistry, School of Chemistry and Chemical Engineering, Hainan University, Haikou, 570228, China. dengpeilin@hainanu.edu.cn.
⁴ Key Laboratory of Electrochemical Energy Storage and Energy Conversion of Hainan Province, School of Chemistry and Chemical Engineering, Hainan Normal University, Haikou, 571158, China.
⁵ College of Marine Science & Technology, Hainan Tropical Ocean University, Sanya, 572022, China.
⁶ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China. lingu@mail.tsinghua.edu.cn.
⁷ School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China. lingu@mail.tsinghua.edu.cn.
⁸ School of Marine Science and Engineering, Hainan Provincial Key Lab of Fine Chemistry, School of Chemistry and Chemical Engineering, Hainan University, Haikou, 570228, China. tianxl@hainanu.edu.cn.
⁹ Guangzhou Key Laboratory of Clean Transportation Energy Chemistry, Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, China. Liuqb@gdut.edu.cn.

^# Contributed equally.

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_xAu_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 Pd₃Au₁ 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.

Abstract

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