High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst

Shuxing Bai; Fangfang Liu; Bolong Huang; Fan Li; Haiping Lin; Tong Wu; Mingzi Sun; Jianbo Wu; Qi Shao; Yong Xu; Xiaoqing Huang

doi:10.1038/s41467-020-14742-x

High-efficiency direct methane conversion to oxygenates on a cerium dioxide nanowires supported rhodium single-atom catalyst

Nat Commun. 2020 Feb 19;11(1):954. doi: 10.1038/s41467-020-14742-x.

Authors

Shuxing Bai^#¹, Fangfang Liu^#², Bolong Huang^#³, Fan Li⁴, Haiping Lin², Tong Wu³, Mingzi Sun³, Jianbo Wu^{5

6}, Qi Shao¹, Yong Xu⁷, Xiaoqing Huang⁸

Affiliations

¹ College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu, 215123, China.
² Institute of Functional Nano&Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Jiangsu, 215123, China.
³ Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, China.
⁴ State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
⁵ State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China. jianbowu@sjtu.edu.cn.
⁶ Center of Hydrogen Science, Shanghai Jiao Tong University, Shanghai, 200240, China. jianbowu@sjtu.edu.cn.
⁷ Institute of Functional Nano&Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Jiangsu, 215123, China. xuy@suda.edu.cn.
⁸ College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Jiangsu, 215123, China. hxq006@suda.edu.cn.

^# Contributed equally.

Abstract

Direct methane conversion (DMC) to high value-added products is of significant importance for the effective utilization of CH₄ to combat the energy crisis. However, there are ongoing challenges in DMC associated with the selective C-H activation of CH₄. The quest for high-efficiency catalysts for this process is limited by the current drawbacks including poor activity and low selectivity. Here we show a cerium dioxide (CeO₂) nanowires supported rhodium (Rh) single-atom (SAs Rh-CeO₂ NWs) that can serve as a high-efficiency catalyst for DMC to oxygenates (i.e., CH₃OH and CH₃OOH) under mild conditions. Compared to Rh/CeO₂ nanowires (Rh clusters) prepared by a conventional wet-impregnation method, CeO₂ nanowires supported Rh single-atom exhibits 6.5 times higher of the oxygenates yield (1231.7 vs. 189.4 mmol g_Rh^-1 h^-1), which largely outperforms that of the reported catalysts in the same class. This work demonstrates a highly efficient DMC process and promotes the research on Rh single-atom catalysts in heterogeneous catalysis.