Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst
Abstract
Electrochemically converting nitrate, a widespread water pollutant, back to valuable ammonia is a green and delocalized route for ammonia synthesis, and can be an appealing and supplementary alternative to the Haber-Bosch process. However, as there are other nitrate reduction pathways present, selectively guiding the reaction pathway towards ammonia is currently challenged by the lack of efficient catalysts. Here we report a selective and active nitrate reduction to ammonia on Fe single atom catalyst, with a maximal ammonia Faradaic efficiency of ~ 75% and a yield rate of up to ~ 20,000 μg h–1 mgcat.–1 (0.46 mmol h–1 cm–2). Our Fe single atom catalyst can effectively prevent the N-N coupling step required for N2 due to the lack of neighboring metal sites, promoting ammonia product selectivity. Density functional theory calculations reveal the reaction mechanisms and the potential limiting steps for nitrate reduction on atomically dispersed Fe sites.
- Authors:
-
[1];
[3];
[1];
[4];
[1];
[4];
[1];
[2];
[2];
[1]
- Rice Univ., Houston, TX (United States)
- Univ. of Calgary, AB (Canada)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Canadian Light Sources, Inc., Saskatoon, SK (Canada); Univ. of Saskatchewan, Saskatoon, SK (Canada)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Welch Foundation
- OSTI Identifier:
- 1787929
- Grant/Contract Number:
- AC05-00OR22725; NEWT EEC 1449500; C-2051-20200401
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 12; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Citation Formats
Wu, Zhen-Yu, Karamad, Mohammadreza, Yong, Xue, Huang, Qizheng, Cullen, David A., Zhu, Peng, Xia, Chuan, Xiao, Qunfeng, Shakouri, Mohsen, Chen, Feng-Yang, Kim, Jung Yoon, Xia, Yang, Heck, Kimberly, Hu, Yongfeng, Wong, Michael S., Li, Qilin, Gates, Ian, Siahrostami, Samira, and Wang, Haotian. Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst. United States: N. p., 2021.
Web. doi:10.1038/s41467-021-23115-x.
Wu, Zhen-Yu, Karamad, Mohammadreza, Yong, Xue, Huang, Qizheng, Cullen, David A., Zhu, Peng, Xia, Chuan, Xiao, Qunfeng, Shakouri, Mohsen, Chen, Feng-Yang, Kim, Jung Yoon, Xia, Yang, Heck, Kimberly, Hu, Yongfeng, Wong, Michael S., Li, Qilin, Gates, Ian, Siahrostami, Samira, & Wang, Haotian. Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst. United States. https://doi.org/10.1038/s41467-021-23115-x
Wu, Zhen-Yu, Karamad, Mohammadreza, Yong, Xue, Huang, Qizheng, Cullen, David A., Zhu, Peng, Xia, Chuan, Xiao, Qunfeng, Shakouri, Mohsen, Chen, Feng-Yang, Kim, Jung Yoon, Xia, Yang, Heck, Kimberly, Hu, Yongfeng, Wong, Michael S., Li, Qilin, Gates, Ian, Siahrostami, Samira, and Wang, Haotian. Mon .
"Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst". United States. https://doi.org/10.1038/s41467-021-23115-x. https://www.osti.gov/servlets/purl/1787929.
@article{osti_1787929,
title = {Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst},
author = {Wu, Zhen-Yu and Karamad, Mohammadreza and Yong, Xue and Huang, Qizheng and Cullen, David A. and Zhu, Peng and Xia, Chuan and Xiao, Qunfeng and Shakouri, Mohsen and Chen, Feng-Yang and Kim, Jung Yoon and Xia, Yang and Heck, Kimberly and Hu, Yongfeng and Wong, Michael S. and Li, Qilin and Gates, Ian and Siahrostami, Samira and Wang, Haotian},
abstractNote = {Electrochemically converting nitrate, a widespread water pollutant, back to valuable ammonia is a green and delocalized route for ammonia synthesis, and can be an appealing and supplementary alternative to the Haber-Bosch process. However, as there are other nitrate reduction pathways present, selectively guiding the reaction pathway towards ammonia is currently challenged by the lack of efficient catalysts. Here we report a selective and active nitrate reduction to ammonia on Fe single atom catalyst, with a maximal ammonia Faradaic efficiency of ~ 75% and a yield rate of up to ~ 20,000 μg h–1 mgcat.–1 (0.46 mmol h–1 cm–2). Our Fe single atom catalyst can effectively prevent the N-N coupling step required for N2 due to the lack of neighboring metal sites, promoting ammonia product selectivity. Density functional theory calculations reveal the reaction mechanisms and the potential limiting steps for nitrate reduction on atomically dispersed Fe sites.},
doi = {10.1038/s41467-021-23115-x},
journal = {Nature Communications},
number = 1,
volume = 12,
place = {United States},
year = {Mon May 17 00:00:00 EDT 2021},
month = {Mon May 17 00:00:00 EDT 2021}
}
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