Revealing the Role of Phase Structures of Bimetallic Nanocatalysts in the Oxygen Reduction Reaction
Abstract
The ability to tune the atomic-level structure of alloy nanoparticles (NPs) is necessary for the design and preparation of active and stable catalysts for fuel cell reactions such as the oxygen reduction reaction (ORR), which is highly sensitive to the structure of the catalysts. We report here structurally tunable PdCu nanoparticle catalysts for the ORR obtained by varying the thermochemical treatment parameters. The phase type and the atomic structure of the nanoalloy catalysts strongly depend on the thermochemical treatment temperature and atmosphere, especially at low temperatures. While PdCu nanoalloys feature both body-centered cubic (bcc) and face-centered cubic (fcc) phase structures, a pure fcc structure, prepared by unusually low thermochemical treatment temperature, showed the highest catalytic activity for ORR. This was evidenced by a mass activity of eight times higher than that of commercial Pd catalyst. This activity enhancement was shown to be linked to the nanostructural tuning between fcc and bcc structures, as supported by systematic characterization using X-ray diffraction coupled with pair distribution function analysis. The impact of phase structure on the catalytic properties of the nanocatalyst is further substantiated by computational modeling based on density functional theory. Our results provide a fresh insight into the nanostructure-activity correlation atmore »
- Authors:
-
[4];
[5];
[2]
- Tianjin Univ. (China); State Univ. of New York (SUNY), Binghamton, NY (United States)
- State Univ. of New York (SUNY), Binghamton, NY (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Central Michigan Univ., Mount Pleasant, MI (United States)
- Tianjin Univ. (China); Southern Illinois Univ., Carbondale, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1493759
- Grant/Contract Number:
- AC02-06CH11357; SC0006877
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 12; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; bimetallic nanocatalysts; fuel cells; nanocrystal structure; oxygen reduction reaction; palladium-copper alloy
Citation Formats
Wu, Zhi-Peng, Shan, Shiyao, Xie, Zhi-Hui, Kang, Ning, Park, Keonwoo, Hopkins, Emma, Yan, Shan, Sharma, Anju, Luo, Jin, Wang, Jie, Petkov, Valeri, Wang, Lichang, and Zhong, Chuan-Jian. Revealing the Role of Phase Structures of Bimetallic Nanocatalysts in the Oxygen Reduction Reaction. United States: N. p., 2018.
Web. doi:10.1021/acscatal.8b03106.
Wu, Zhi-Peng, Shan, Shiyao, Xie, Zhi-Hui, Kang, Ning, Park, Keonwoo, Hopkins, Emma, Yan, Shan, Sharma, Anju, Luo, Jin, Wang, Jie, Petkov, Valeri, Wang, Lichang, & Zhong, Chuan-Jian. Revealing the Role of Phase Structures of Bimetallic Nanocatalysts in the Oxygen Reduction Reaction. United States. https://doi.org/10.1021/acscatal.8b03106
Wu, Zhi-Peng, Shan, Shiyao, Xie, Zhi-Hui, Kang, Ning, Park, Keonwoo, Hopkins, Emma, Yan, Shan, Sharma, Anju, Luo, Jin, Wang, Jie, Petkov, Valeri, Wang, Lichang, and Zhong, Chuan-Jian. Fri .
"Revealing the Role of Phase Structures of Bimetallic Nanocatalysts in the Oxygen Reduction Reaction". United States. https://doi.org/10.1021/acscatal.8b03106. https://www.osti.gov/servlets/purl/1493759.
@article{osti_1493759,
title = {Revealing the Role of Phase Structures of Bimetallic Nanocatalysts in the Oxygen Reduction Reaction},
author = {Wu, Zhi-Peng and Shan, Shiyao and Xie, Zhi-Hui and Kang, Ning and Park, Keonwoo and Hopkins, Emma and Yan, Shan and Sharma, Anju and Luo, Jin and Wang, Jie and Petkov, Valeri and Wang, Lichang and Zhong, Chuan-Jian},
abstractNote = {The ability to tune the atomic-level structure of alloy nanoparticles (NPs) is necessary for the design and preparation of active and stable catalysts for fuel cell reactions such as the oxygen reduction reaction (ORR), which is highly sensitive to the structure of the catalysts. We report here structurally tunable PdCu nanoparticle catalysts for the ORR obtained by varying the thermochemical treatment parameters. The phase type and the atomic structure of the nanoalloy catalysts strongly depend on the thermochemical treatment temperature and atmosphere, especially at low temperatures. While PdCu nanoalloys feature both body-centered cubic (bcc) and face-centered cubic (fcc) phase structures, a pure fcc structure, prepared by unusually low thermochemical treatment temperature, showed the highest catalytic activity for ORR. This was evidenced by a mass activity of eight times higher than that of commercial Pd catalyst. This activity enhancement was shown to be linked to the nanostructural tuning between fcc and bcc structures, as supported by systematic characterization using X-ray diffraction coupled with pair distribution function analysis. The impact of phase structure on the catalytic properties of the nanocatalyst is further substantiated by computational modeling based on density functional theory. Our results provide a fresh insight into the nanostructure-activity correlation at the atomic scale, which has significant implications for the design, synthesis, and processing of highly-active nanoalloy catalysts.},
doi = {10.1021/acscatal.8b03106},
journal = {ACS Catalysis},
number = 12,
volume = 8,
place = {United States},
year = {Fri Nov 02 00:00:00 EDT 2018},
month = {Fri Nov 02 00:00:00 EDT 2018}
}
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