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A facile strategy to prepare FeNx decorated PtFe intermetallic with excellent acidic oxygen reduction reaction
Xue Liu1, Qianli Xing2, Jie Song1
1School of Materials Science and Engineering, China University of Petroleum (East China), Qingdao 266580, China.
Abstract:
The construction of low-Pt-content intermetallic on carbon supports has been verified as a promising method to promote the activity of the oxygen reduction reaction (ORR). In this study, we have developed a simple and effective strategy to obtain a well-designed CNT-PtFe-PPy precursor. This precursor contains modulated Pt- and Fe-based content dispersed in polypyrrole (PPy) chain segments, which are in-situ generated on the templates of carbon nanotubes (CNTs). Subsequent pyrolysis of the CNT-PtFe-PPy precursor produces a CNT-PtFe@FeNC catalyst, which contains both Fe-Nx and PtFe intermetallic active sites. Due to the highly efficient dispersion of active species, the CNT-PtFe@FeNC electrocatalyst displays a 9.5 times higher specific activity (SA) and 8.5 times higher mass activity (MA) than those of a commercial Pt/C catalyst in a 0.1 M HClO4 solution. Additionally, these results, combined with excellent durability (the SA and MA maintained 94 % and 91 % of initial activity after a 10-k cycle accelerated durability test), represent among the best performance achieved so far for Pt-based ORR electrocatalysts. Furthermore, density functional theory (DFT) calculations revealed that the presence of Fe-N4 species reduces the adsorption energy between the PtFe intermetallic compound and OH*, accelerating the ORR process.
