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Abstract:
The insufficient durability of Pt-based catalysts and the sluggish kinetics of oxygen reduction reaction (ORR) is hampering the development of proton exchange membrane fuel cells (PEMFCs) for commercialization. Herein, a single atom Ti-modified activated nitrogen-doped porous carbon (Ti-a-NPC) is designed to equalize O2-activation/*OH-removal through regulating the charge rearrangement of ultra-small L12-Pt3Co for efficient and durable oxygen reduction. The Ti single-atom modified in the surface/pore of Ti-a-NPC can anchor the Pt-based intermetallic nanoparticles (NPs) not only guarantees Pt-based intermetallics' ultra-fine size (approximate to 2.62 nm) but also maintains Pt-based intermetallics during ORR process. The enhanced catalyst (L12-Pt3Co/Ti-a-NPC) achieves 11-fold mass activity (1.765 A mgPt-1) compared to commercial Pt/C. Notably, after 30 000 cycles of accelerated durability tests, the mass activity of the L12-Pt3Co/Ti-a-NPC only decreased by 3.7%, while that of commercial Pt/C decreased by 37.1%. Rationalized by theoretical simulation, the introduction of Ti atoms can form charge channels between L12-Pt3Co NPs and Ti-a-NPC, accelerating the charge transfer in the ORR process. Furthermore, the charge of L12-Pt3Co will accumulate to Ti atoms and buffer the electron transfer of L12-Pt3Co to the N atoms, thus optimizing the adsorption performance of the active site to the oxygen-containing intermediate and improving the intrinsic activity of the catalyst. The single-atom Ti synergizes with the confinement effect of Ti-a-NPC not only restricting the size increase of Pt-based intermetallics during the ordering process (average size 2.6 nm) but also inhibiting the shedding and migration of Pt-based intermetallics under fuel cell operating conditions. The charge of ultra-small L12-Pt3Co is regulated by single atom Ti to equalize O2-activation/*OH-removal for efficient oxygen reduction. image
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ADVANCED FUNCTIONAL MATERIALS
ISSN: 1616-301X
Year: 2024
Issue: 44
Volume: 34
1 8 . 5 0 0
JCR@2023
Cited Count:
SCOPUS Cited Count: 4
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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