Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

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

doi:10.1038/s41467-021-23115-x

Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

Journal Article · Mon May 17 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-23115-x· OSTI ID:1787929

^[1]; Karamad, Mohammadreza ^[2]; Yong, Xue ^[2]; Huang, Qizheng ^[1]; ^[3]; ^[1]; Xia, Chuan ^[1]; Xiao, Qunfeng ^[4]; ^[4]; ^[1]; Kim, Jung Yoon ^[1]; Xia, Yang ^[1]; Heck, Kimberly ^[1]; ^[4]; ^[1]; Li, Qilin ^[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)

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Welch Foundation

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1787929

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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