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 () and Haotian Wang ()
Additional contact information
Zhen-Yu Wu: Rice University
Mohammadreza Karamad: University of Calgary
Xue Yong: University of Calgary
Qizheng Huang: Rice University
David A. Cullen: Oak Ridge National Laboratory
Peng Zhu: Rice University
Chuan Xia: Rice University
Qunfeng Xiao: University of Saskatchewan
Mohsen Shakouri: University of Saskatchewan
Feng-Yang Chen: Rice University
Jung Yoon (Timothy) Kim: Rice University
Yang Xia: Rice University
Kimberly Heck: Rice University
Yongfeng Hu: University of Saskatchewan
Michael S. Wong: Rice University
Qilin Li: Rice University
Ian Gates: University of Calgary
Samira Siahrostami: University of Calgary
Haotian Wang: Rice University

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: 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.

Date: 2021
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Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-23115-x

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DOI: 10.1038/s41467-021-23115-x

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