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Reduction of N₂ to Ammonia by Phosphate Molten Salt and Li Electrode: Proof of Concept Using Quantum Mechanics

Musgrave, Charles B., III and Morozov, Sergey and Schinski, William L. and Goddard, William A., III (2021) Reduction of N₂ to Ammonia by Phosphate Molten Salt and Li Electrode: Proof of Concept Using Quantum Mechanics. Journal of Physical Chemistry Letters, 12 (6). pp. 1696-1701. ISSN 1948-7185. https://resolver.caltech.edu/CaltechAUTHORS:20210210-082941054

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Abstract

Electrochemical routes provide an attractive alternative to the Haber–Bosch process for cheaper and more efficient ammonia (NH₃) synthesis from N₂ while avoiding the onerous environmental impact of the Haber–Bosch process. We prototype a strategy based on a eutectic mixture of phosphate molten salt. Using quantum-mechanics (QM)-based reactive molecular dynamics, we demonstrate that lithium nitride (Li₃N) produced from the reduction of nitrogen gas (N₂) by a lithium electrode can react with the phosphate molten salt to form ammonia. We extract reaction kinetics of the various steps from QM to identify conditions with favorable reaction rates for N₂ reduction by a porous lithium electrode to form Li₃N followed by protonation from phosphate molten salt (Li₂HPO₄–LiH₂PO₄ mixture) to selectively form NH₃.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1021/acs.jpclett.0c03467DOIArticle
ORCID:
AuthorORCID
Musgrave, Charles B., III0000-0002-3432-0817
Morozov, Sergey0000-0001-6226-5811
Goddard, William A., III0000-0003-0097-5716
Alternate Title:Reduction of N2 to Ammonia by Phosphate Molten Salt and Li Electrode: Proof of Concept Using Quantum Mechanics
Additional Information:© 2021 American Chemical Society. Received: November 22, 2020; Accepted: February 3, 2021; Published: February 9, 2021. This material is based on work performed by the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award Number DE-SC0021266. The authors declare no competing financial interest.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0021266
Other Numbering System:
Other Numbering System NameOther Numbering System ID
WAG1410
Issue or Number:6
Record Number:CaltechAUTHORS:20210210-082941054
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210210-082941054
Official Citation:Reduction of N₂ to Ammonia by Phosphate Molten Salt and Li Electrode: Proof of Concept Using Quantum Mechanics. Charles B. Musgrave, Sergey Morozov, William L. Schinski, and William A. Goddard The Journal of Physical Chemistry Letters 2021 12 (6), 1696-1701. DOI: 10.1021/acs.jpclett.0c03467
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:107981
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:10 Feb 2021 17:05
Last Modified:27 Mar 2021 08:14

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