Journal
ACS CATALYSIS
Volume 12, Issue 15, Pages 8848-8856Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c01052
Keywords
oxygen reduction reaction; Pt catalyst; interstitial B doping; durability; dimethylamine borane
Categories
Funding
- National Key Research and Development Program of China [2021YFB4001300]
- NSFC [21733004, 22122202]
- 973 Program of MOST [2015CB932303]
- International Cooperation Program of STCSM [17520711200]
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This study investigates the use of interstitial B-doping in the Pt lattice to design a durable and active Pt-B/C catalyst, which enhances the catalyst's activity and durability by regulating the electronic structure of surface Pt sites. Experimental results demonstrate that the synthesized Pt-B/C catalyst outperforms commercial Pt/C(com) in terms of activity and durability, showing better performance in PEMFCs.
The dissolution of M in currently popular Pt-M alloy catalysts (M = Co, Ni, and Fe) during the oxygen reduction reaction (ORR) may deter their wide application in proton exchange membrane fuel cells (PEMFCs). In this work, interstitial B-doping in the Pt lattice is instead used to design a durable and active ORR catalyst, by taking advantage of its unique regulation of the electronic structure of surface Pt sites. 3 nm Pt-B nanoparticles on carbon black (Pt-B/C) are obtained using dimethylamine borane (DMAB) as a reductant and the B source in a mixed H2O-ethylene glycol precursor solution. The formation of the B-doped Pt catalyst is verified by inductively coupled plasma-atomic emission spectrometry, X-ray diffractometry, and spherical aberration-corrected scanning transmission electron microscopy. Both half-cell and single-cell tests indicate that the as-synthesized Pt-B/C catalyst outperforms the commercial Pt/C(com) in terms of activity and durability. In particular, the Pt-B/C-based PEMFC exhibits an initial maximum power density 1.24 times as high as the Pt/C(com)-based one under otherwise same conditions, with a 15% decay for the former versus a 45% decay for the latter after 30 000 cycles of the accelerated degradation test (ADT). Comparative DFT calculations on B-doped and undoped Pt(111) surfaces reveal that the lowered Pt d-band center and the strong interaction of Pt-B bonding weaken the binding of OH and O species to surface Pt sites and lessen oxidative disruption of surface Pt atoms. This interstitial metalloid doping in conjunction with the simple and scalable synthesis protocol enables the Pt-B/C to be a competitive ORR catalyst for the PEMFCs.
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