Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

Zhen Yu Wu; Mohammadreza Karamad; Xue Yong; Qizheng Huang; David A. Cullen; Peng Zhu; Chuan Xia; Qunfeng Xiao; Mohsen Shakouri; Feng Yang Chen; Jung Yoon (Timothy) Kim; Yang Xia; Kimberly Heck; Yongfeng Hu; Michael S. Wong; Qilin Li; Ian Gates; Samira Siahrostami; Haotian Wang

doi:10.1038/s41467-021-23115-x

Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

Zhen Yu Wu, Mohammadreza Karamad, Xue Yong, Qizheng Huang, David A. Cullen, Peng Zhu, Chuan Xia, Qunfeng Xiao, Mohsen Shakouri, Feng Yang Chen, Jung Yoon (Timothy) Kim, Yang Xia, Kimberly Heck, Yongfeng Hu, Michael S. Wong, Qilin Li, Ian Gates, Samira Siahrostami, Haotian Wang

Materials MicroAnalysis

Research output: Contribution to journal › Article › peer-review

889 Scopus citations

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 mg_cat.⁻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.

Original language	English
Article number	2870
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-23115-x
State	Published - Dec 1 2021

Funding

This work was supported by Rice University, the National Science Foundation Nano-systems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT EEC 1449500), and the Welch Foundation Research Grant (C-2051-20200401). H.W. is a CIFAR Azrieli Global Scholar in the Bio-inspired Solar Energy Program. S.S. acknowledges the support from the University of Calgary’s Canada First Research Excellence Fund Program, the Global Research Initiative in Sustainable Low Carbon Unconventional Resources. Aberration-corrected STEM-EELS was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. The authors acknowledge Prof. H.W. Liang and M.X. Chen for XAS measurement and data analysis.

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Wu, Z. Y., Karamad, M., Yong, X., Huang, Q., Cullen, D. A., Zhu, P., Xia, C., Xiao, Q., Shakouri, M., Chen, F. Y., Kim, J. Y., Xia, Y., Heck, K., Hu, Y., Wong, M. S., Li, Q., Gates, I., Siahrostami, S., & Wang, H. (2021). Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst. Nature Communications, 12(1), Article 2870. https://doi.org/10.1038/s41467-021-23115-x

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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.",

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AU - Zhu, Peng

AU - Xia, Chuan

AU - Xiao, Qunfeng

AU - Shakouri, Mohsen

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AU - Kim, Jung Yoon (Timothy)

AU - Xia, Yang

AU - Heck, Kimberly

AU - Hu, Yongfeng

AU - Wong, Michael S.

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AU - Gates, Ian

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Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

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