High-loaded sub-6 nm Pt1Co1 intermetallic compounds with high-efficient performance expression in PEMFCs

Energy and Environmental Science(2021)

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摘要
High-loaded oxygen reduction reaction (ORR) Pt intermetallic compounds with high performance expression under PEMFC operating conditions are prerequisite for practical application. Nevertheless, high metal-loading would lead to the severe agglomeration and nonuniformity of nanoparticles, imposing an enormous challenge on efficient synthesis. Herein we present a cobalt oxide aided structural evolution strategy to controllably synthesize high-loaded (44.7 wt%) sub-6 nm Pt1Co1 intermetallic compound with Pt-rich shell (Pt1Co1-IMC@Pt). Experiments and theory explicitly reveal that the ordered arrangement of Pt-Co atoms endows surface Pt with lowered d band centre and enhanced oxidation-resistance of Pt/Co sites, thus simultaneously boosting the ORR activity and durability. The preeminent intrinsic ORR activity on an optimized catalyst reaches a mass activity as high as 0.53 A mg(Pt)-1 @0.90V/RHE (MA@0.9 V) in rotating disk electrode measurement. PEMFCs with such a catalyst deliver the record-high power density (2.30/1.23 Wcm-2 under H2-air/O2 conditions at 80 oC) and extraordinary stability, ranking the highest fuel cell performance among the Pt-based electrocatalysts. Significantly, the MA@0.9 V calculated from fuel cell attains 0.46 A mg(Pt)-1, exceeding the 2020 DOE target (0.44 A mg(Pt)-1) and very close to the intrinsic value, definitely confirming the superiority of high-loaded Pt1Co1-IMC@Pt/C in activity expression under fuel cell conditions. This study paves a new way for the future practical application of low-Pt catalysts in PEMFCs.
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