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author:

Zichen Wang (Zichen Wang.) [1] | Suhao Chen (Suhao Chen.) [2] | Wei Wu (Wei Wu.) [3] | Runzhe Chen (Runzhe Chen.) [4] | Yu Zhu (Yu Zhu.) [5] | Haoran Jiang (Haoran Jiang.) [6] | Liyue Yu (Liyue Yu.) [7] | Niancai Cheng (Niancai Cheng.) [8]

Abstract:

The sluggish kinetics of oxygen reduction reaction (ORR) and unsatisfactory durability of Pt‐based catalysts are severely hindering the commercialization of proton‐exchange‐membrane fuel cells (PEMFCs). In this work, the lattice compressive strain of Pt‐skins imposed by Pt‐based intermetallic cores is tailored for highly effective ORR through the confinement effect of the activated nitrogen‐doped porous carbon (a‐NPC). The modulated pores of a‐NPC not only promote Pt‐based intermetallics with ultrasmall size (average size of <4 nm), but also efficiently stabilizes intermetallic nanoparticles and sufficient exposure of active sites during the ORR process. The optimized catalyst (L12‐Pt3Co@ML‐Pt/NPC10) achieves excellent mass activity (1.72 A mgPt−1) and specific activity (3.49 mA cmPt−2), which are 11‐ and 15‐fold that of commercial Pt/C, respectively. Besides, owing to the confinement effect of a‐NPC and protection of Pt‐skins, L12‐Pt3Co@ML‐Pt/NPC10 retains 98.1% mass activity after 30 000 cycles, and even 95% for 100 000 cycles, while Pt/C retains only 51.2% for 30 000 cycles. Rationalized by density functional theory, compared with other metals (Cr, Mn, Fe, and Zn), L12‐Pt3Co closer to the top of “volcano” induces a more suitable compressive strain and electronic structure on Pt‐skin, leading to an optimal oxygen adsorption energy and a remarkable ORR performance.

Keyword:

compressive strains confinement effects fuel cells intermetallics oxygen reduction reaction

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Advanced Materials

ISSN: 0935-9648

Year: 2023

Issue: 36

Volume: 35

Page: n/a-n/a

2 7 . 4

JCR@2023

2 7 . 4 0 0

JCR@2023

JCR Journal Grade:1

CAS Journal Grade:1

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SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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