Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts
Abstract
Abstract Atomically dispersed and nitrogen coordinated single metal sites (M‐N‐C, M=Fe, Co, Ni, Mn) are the popular platinum group‐metal (PGM)‐free catalysts for many electrochemical reactions. Traditional wet‐chemistry catalyst synthesis often requires complex procedures with unsatisfied reproducibility and scalability. Here, we report a facile chemical vapor deposition (CVD) strategy to synthesize the promising M‐N‐C catalysts. The deposition of gaseous 2‐methylimidazole onto M‐doped ZnO substrates, followed by an in situ thermal activation, effectively generated single metal sites well dispersed into porous carbon. In particular, an optimal CVD‐derived Fe‐N‐C catalyst exclusively contains atomically dispersed FeN 4 sites with increased Fe loading relative to other catalysts from wet‐chemistry synthesis. The catalyst exhibited outstanding oxygen‐reduction activity in acidic electrolytes, which was further studied in proton‐exchange membrane fuel cells with encouraging performance.
- Authors:
-
[4];
[4];
[1]
- Univ. at Buffalo, NY (United States)
- Oregon State Univ., Corvallis, OR (United States)
- Northwestern Univ., Evanston, IL (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; National Science Foundation (NSF); USDOE
- OSTI Identifier:
- 1772863
- Alternate Identifier(s):
- OSTI ID: 1786196
- Grant/Contract Number:
- AC05-00OR22725; EE0008076; EE0008417; CBET-1604392; CBET-1804326; EE0008075, DE-EE0008076, and DE-EE0008417
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 59; Journal Issue: 48; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; single metal sites; chemical vapor deposition; Fe-N-C; oxygen reduction reaction; electrocatalysis.
Citation Formats
Liu, Shengwen, Wang, Maoyu, Yang, Xiaoxuan, Shi, Qiurong, Qiao, Zhi, Lucero, Marcos, Ma, Qing, More, Karren L., Cullen, David A., Feng, Zhenxing, and Wu, Gang. Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts. United States: N. p., 2019.
Web. doi:10.1002/anie.202009331.
Liu, Shengwen, Wang, Maoyu, Yang, Xiaoxuan, Shi, Qiurong, Qiao, Zhi, Lucero, Marcos, Ma, Qing, More, Karren L., Cullen, David A., Feng, Zhenxing, & Wu, Gang. Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts. United States. https://doi.org/10.1002/anie.202009331
Liu, Shengwen, Wang, Maoyu, Yang, Xiaoxuan, Shi, Qiurong, Qiao, Zhi, Lucero, Marcos, Ma, Qing, More, Karren L., Cullen, David A., Feng, Zhenxing, and Wu, Gang. Wed .
"Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts". United States. https://doi.org/10.1002/anie.202009331. https://www.osti.gov/servlets/purl/1772863.
@article{osti_1772863,
title = {Chemical Vapor Deposition for Atomically Dispersed and Nitrogen Coordinated Single Metal Site Catalysts},
author = {Liu, Shengwen and Wang, Maoyu and Yang, Xiaoxuan and Shi, Qiurong and Qiao, Zhi and Lucero, Marcos and Ma, Qing and More, Karren L. and Cullen, David A. and Feng, Zhenxing and Wu, Gang},
abstractNote = {Abstract Atomically dispersed and nitrogen coordinated single metal sites (M‐N‐C, M=Fe, Co, Ni, Mn) are the popular platinum group‐metal (PGM)‐free catalysts for many electrochemical reactions. Traditional wet‐chemistry catalyst synthesis often requires complex procedures with unsatisfied reproducibility and scalability. Here, we report a facile chemical vapor deposition (CVD) strategy to synthesize the promising M‐N‐C catalysts. The deposition of gaseous 2‐methylimidazole onto M‐doped ZnO substrates, followed by an in situ thermal activation, effectively generated single metal sites well dispersed into porous carbon. In particular, an optimal CVD‐derived Fe‐N‐C catalyst exclusively contains atomically dispersed FeN 4 sites with increased Fe loading relative to other catalysts from wet‐chemistry synthesis. The catalyst exhibited outstanding oxygen‐reduction activity in acidic electrolytes, which was further studied in proton‐exchange membrane fuel cells with encouraging performance.},
doi = {10.1002/anie.202009331},
journal = {Angewandte Chemie (International Edition)},
number = 48,
volume = 59,
place = {United States},
year = {Wed Aug 21 00:00:00 EDT 2019},
month = {Wed Aug 21 00:00:00 EDT 2019}
}
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