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

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. The preferential oxidation of CO (PROX) in hydrogen is a promising solution for hydrogen purification. Here the authors report a novel bimetallic Pt-Fe catalyst with ultralow metal loading which delivers excellent catalytic activity and selectivity in PROX, while maintains good stability for a long period.

Automated summary

This study reports a novel bimetallic Pt-Fe catalyst with ultralow metal loading, which shows excellent catalytic activity and selectivity in the preferential oxidation of CO (PROX) in hydrogen. The fully-exposed Pt-Fe clusters on the defective graphene surface can achieve complete elimination of CO and maintain good stability for a long period. The construction of fully-exposed bimetallic Pt-Fe catalysts with maximized atomic efficiency and abundant interfacial sites facilitates oxygen activation and CO oxidation, leading to excellent reactivity in practical applications.