Journal
ACS CATALYSIS
Volume 11, Issue 1, Pages 184-192Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.0c04021
Keywords
oxygen reduction reaction; rhombohedral ordered intermetallics; core shell; N-doping; PtCu nanocatalyst
Categories
Funding
- U.S. Department of Energy [DE-SC0012704]
- National Science Foundation [CHE-1900401]
- Integrated Mesoscale Architectures for Sustainable Catalysis (IMASC), an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0012573]
- U.S. DOE Office of Science Facilities, at Brookhaven National Laboratory [DE-SC0012704]
- Synchrotron Catalysis Consortium (U.S. DOE, Office of Basic Energy Sciences) [DE-SC0012335]
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The study presents the synthesis of an L1(1)-ordered PtCu catalyst for the oxygen reduction reaction (ORR), demonstrating that nitrogen doping can enhance the activity and stability of the catalyst. The research shows that in acidic media, the ORR mass and specific activities of the N-doped, rhombohedral ordered PtCu catalyst achieve nearly 5-fold and 4-fold enhancement, respectively, compared to commercial Pt/C.
Low platinum-group-metal (PGM) ordered intermetallic catalysts have been considered one of the most promising candidates for catalyzing the oxygen reduction reaction (ORR) in fuel cells, but achieving the desired performances in terms of activity, durability, and cost is still a grand challenge for the fuel cell research field. While the cubic- and tetragonal-ordered (L1(2) and L1(0) phases) low-PGM nanocatalysts have been investigated extensively and have shown considerably improved durability and activity toward the ORR, so far, little is known about rhombohedral ordered L1(1) catalysts. We report the synthesis of an L1(1)-ordered PtCu catalyst for the ORR. We demonstrate that by applying nitrogen (N) doping through a thermal treatment in an NH3 gas, the activity and stability of the N-doped, rhombohedral ordered PtCu catalyst can be further enhanced, and the ORR mass and specific activities achieve nearly 5-fold and 4-fold enhancement in acidic media, respectively, relative to those of commercial Pt/C. In situ synchrotron X-ray absorption and pair-distribution-function measurements reveal that both the formation of the ordered intermetallic structure and N-doping synergistically improve the corrosion resistance of the PtCu catalyst by lowering the Cu diffusivity and introduce a compressive strain effect regulating the adsorption of oxygenated species on the Pt surface, thus accounting for the improved ORR kinetics.
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