Fully-exposed Pt-Fe cluster for efficient preferential oxidation of CO towards hydrogen purification

Zhimin Jia; Xuetao Qin; Yunlei Chen; Xiangbin Cai; Zirui Gao; Mi Peng; Fei Huang; Dequan Xiao; Xiaodong Wen; Ning Wang; Zheng Jiang; Wu Zhou; Hongyang Liu; Ding Ma

doi:10.1038/s41467-022-34674-y

Fully-exposed Pt-Fe cluster for efficient preferential oxidation of CO towards hydrogen purification

Nat Commun. 2022 Nov 10;13(1):6798. doi: 10.1038/s41467-022-34674-y.

Authors

Zhimin Jia^#^{1

2}, Xuetao Qin^#³, Yunlei Chen^#^{4

5}, Xiangbin Cai^#⁶, Zirui Gao³, Mi Peng³, Fei Huang¹, Dequan Xiao⁷, Xiaodong Wen^{4

5}, Ning Wang⁶, Zheng Jiang⁸, Wu Zhou⁹, Hongyang Liu^{10

11}, Ding Ma¹²

Affiliations

¹ Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, P. R. China.
² School of Materials Science and Engineering, University of Science and Technology of China, Shenyang, 110016, P. R. China.
³ College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China.
⁴ University of Chinese Academy of Science, No. 19A Yuanquan Road, Beijing, 100049, P. R. China.
⁵ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, P. R. China.
⁶ Department of Physics and Center for Quantum Materials, Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong SAR, P. R. China.
⁷ Center for Integrative Materials Discovery, Department of Chemistry and Chemical Engineering, University of New Haven, 300 Boston Post Road, West Haven, CT, 06516, USA.
⁸ Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, P. R. China.
⁹ School of Physical Sciences and CAS Center for Excellence in Topological Quantum Computation, University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.
¹⁰ Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, 110016, P. R. China. liuhy@imr.ac.cn.
¹¹ School of Materials Science and Engineering, University of Science and Technology of China, Shenyang, 110016, P. R. China. liuhy@imr.ac.cn.
¹² College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, P. R. China. dma@pku.edu.cn.

^# Contributed equally.

Abstract

Hydrogen is increasingly being discussed as clean energy for the goal of net-zero carbon emissions, applied in the proton-exchange-membrane fuel cells (PEMFC). The preferential oxidation of CO (PROX) in hydrogen is a promising solution for hydrogen purification to avoid catalysts from being poisoned by the trace amount of CO in hydrogen-rich fuel gas. Here, we report the fabrication of a novel bimetallic Pt-Fe catalyst with ultralow metal loading, in which fully-exposed Pt clusters bonded with neighbor atomically dispersed Fe atoms on the defective graphene surface. The fully-exposed PtFe cluster catalyst could achieve complete elimination of CO through PROX reaction and almost 100% CO selectivity, while maintaining good stability for a long period. It has the mass-specific activity of 6.19 (mol_CO)*(g_Pt)^-1*h^-1 at room temperature, which surpasses those reported in literatures. The exhaustive experimental results and theoretical calculations reveal that the construction of fully-exposed bimetallic Pt-Fe cluster catalysts with maximized atomic efficiency and abundant interfacial sites could facilitate oxygen activation on unsaturated Fe species and CO adsorption on electron-rich Pt clusters to hence the probability of CO oxidation, leading to excellent reactivity in practical applications.