Atomic-thick metastable phase RhMo nanosheets for hydrogen oxidation catalysis

Juntao Zhang; Xiaozhi Liu; Yujin Ji; Xuerui Liu; Dong Su; Zhongbin Zhuang; Yu-Chung Chang; Chih-Wen Pao; Qi Shao; Zhiwei Hu; Xiaoqing Huang

doi:10.1038/s41467-023-37406-y

Atomic-thick metastable phase RhMo nanosheets for hydrogen oxidation catalysis

Nat Commun. 2023 Mar 30;14(1):1761. doi: 10.1038/s41467-023-37406-y.

Authors

Juntao Zhang^#¹, Xiaozhi Liu^#², Yujin Ji^#³, Xuerui Liu⁴, Dong Su⁵, Zhongbin Zhuang⁴, Yu-Chung Chang⁶, Chih-Wen Pao⁶, Qi Shao⁷, Zhiwei Hu⁸, Xiaoqing Huang⁹

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China.
² Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
³ Institute of Functional Nano and Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Jiangsu, 215123, China.
⁴ State Key Lab of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, China.
⁵ Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China. dongsu@iphy.ac.cn.
⁶ National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, 30076, Hsinchu, Taiwan.
⁷ College of Chemistry and Chemical Engineering and Materials Science, Soochow University, Jiangsu, 215123, China. qshao@suda.edu.cn.
⁸ Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, Dresden, 01187, Germany.
⁹ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China. hxq006@xmu.edu.cn.

^# Contributed equally.

Abstract

Metastable phase two-dimensional catalysts provide great flexibility for modifying their chemical, physical, and electronic properties. However, the synthesis of ultrathin metastable phase two-dimensional metallic nanomaterials is highly challenging, mainly due to the anisotropic nature of metallic materials and their thermodynamically unstable ground-state. Here, we report free-standing RhMo nanosheets with atomic thickness and a unique core/shell (metastable phase/stable phase) structure. The polymorphic interface between the core region and shell region stabilizes and activates metastable phase catalysts; the RhMo Nanosheets/C shows excellent hydrogen oxidation activity and stability. Specifically, the mass activities of RhMo Nanosheets/C is 6.96 A mg_Rh^-1; this is 21.09 times higher than that of commercial Pt/C (0.33 A mg_Pt^-1). Density functional theory calculations suggest that the interface aids in the dissociation of H₂ and the H species can then spillover to weak H binding sites for desorption, providing excellent hydrogen oxidation activity for RhMo nanosheets. This work advances the highly controlled synthesis of two-dimensional metastable phase noble metals and provides great directions for the design of high-performance catalysts for fuel cells and beyond.