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author:

Wang, Zichen (Wang, Zichen.) [1] | Wu, Wei (Wu, Wei.) [2] | Jiang, Haoran (Jiang, Haoran.) [3] | Chen, Suhao (Chen, Suhao.) [4] | Chen, Runzhe (Chen, Runzhe.) [5] | Zhu, Yu (Zhu, Yu.) [6] | Xiao, Yong (Xiao, Yong.) [7] | Lv, Haifeng (Lv, Haifeng.) [8] | Zhong, Jun (Zhong, Jun.) [9] | Cheng, Niancai (Cheng, Niancai.) [10] (Scholars:程年才)

Indexed by:

EI Scopus SCIE

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

Keyword:

charge rearrangement fuel cells oxygen reduction reaction Pt-based intermetallics Ti single-atom

Community:

  • [ 1 ] [Wang, Zichen]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 2 ] [Wu, Wei]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 3 ] [Jiang, Haoran]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 4 ] [Chen, Suhao]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 5 ] [Chen, Runzhe]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 6 ] [Zhu, Yu]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 7 ] [Xiao, Yong]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 8 ] [Cheng, Niancai]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 9 ] [Lv, Haifeng]Shenzhen Acad Aerosp Technol, PEM Fuel Cell Catalyst Res & Dev Ctr, Shenzhen 518057, Peoples R China
  • [ 10 ] [Zhong, Jun]Soochow Univ, Inst Funct Nano & Soft Mat Lab FUNSOM, Jiangsu Key Lab Adv Negat Carbon Technol, Suzhou 215123, Peoples R China

Reprint 's Address:

  • [Cheng, Niancai]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China;;[Lv, Haifeng]Shenzhen Acad Aerosp Technol, PEM Fuel Cell Catalyst Res & Dev Ctr, Shenzhen 518057, Peoples R China;;[Zhong, Jun]Soochow Univ, Inst Funct Nano & Soft Mat Lab FUNSOM, Jiangsu Key Lab Adv Negat Carbon Technol, Suzhou 215123, Peoples R China;;

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Source :

ADVANCED FUNCTIONAL MATERIALS

ISSN: 1616-301X

Year: 2024

Issue: 44

Volume: 34

1 8 . 5 0 0

JCR@2023

Cited Count:

WoS CC 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

Online/Total:119/10052014
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