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Electrochemical ammonia synthesis via nitrate reduction on Fe single atom catalyst

Zhenyu WuDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAMohammadreza KaramadDepartment of Chemical and Petroleum Engineering, University of Calgary, Calgary, AB, CanadaXue YongDepartment of Chemistry, University of Calgary, Calgary, AB, CanadaQizheng HuangDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USADavid A. CullenCenter for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, TN, USAPeng ZhuDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAChuan XiaDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAQunfeng XiaoCanadian Light Source Inc., University of Saskatchewan, Saskatoon, SK, CanadaMohsen ShakouriCanadian Light Source Inc., University of Saskatchewan, Saskatoon, SK, CanadaFeng-Yang ChenDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAJung Yoon KimDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAXia YangDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAKimberly N. HeckDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAYongfeng HuCanadian Light Source Inc., University of Saskatchewan, Saskatoon, SK, CanadaMichael S. WongDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX, USAQilin LiDepartment of Civil and Environmental Engineering, Rice University, Houston, TX, USAIan D. GatesDepartment of Chemical and Petroleum Engineering, University of Calgary, Calgary, AB, CanadaSamira SiahrostamiDepartment of Chemistry, University of Calgary, Calgary, AB, Canada. [email protected]Haotian WangAzrieli Global Scholar, Canadian Institute for Advanced Research (CIFAR), Toronto, ON, Canada. [email protected]

2021en

ABI

Annotatsiya

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 N 2 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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DOI: 10.1038/s41467-021-23115-x

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