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Title: Catalysts for nitrogen reduction to ammonia

Abstract

We present the production of synthetic ammonia remains dependent on the energy- and capital-intensive Haber-Bosch process. Extensive research in molecular catalysis has demonstrated ammonia production from di-nitrogen, albeit at low production rates. Mechanistic understanding of di-nitrogen reduction to ammonia continues to be delineated through study of molecular catalyst structure, as well as through understanding the naturally-occurring nitrogenase enzyme. The transition to Haber-Bosch alternatives through robust, heterogeneous catalyst surfaces remains an unsolved research challenge. Catalysts for electrochemical reduction of di-nitrogen to ammonia are a specific focus of research, due to the potential to compete with Haber-Bosch and eliminate associated carbon dioxide emissions. However, limited progress has been made, as most electrocatalyst surfaces lack specificity towards nitrogen fixation. Lastly in this review, we discuss the progress of the field in developing a mechanistic understanding of nitrogenase-promoted and molecular catalyst-promoted ammonia synthesis and provide a review of the state-of-the-art and scientific needs for heterogeneous electrocatalysts.

Authors:
 [1];  [1];  [2];  [3];  [4]; ORCiD logo [4];  [3];  [2];  [1]
  1. Univ. of Arkansas, Fayetteville, AR (United States). Ralph E. Martin Department of Chemical Engineering
  2. Case Western Reserve Univ., Cleveland, OH (United States). Department of Chemical and Biomolecular Engineering
  3. Pennsylvania State Univ., University Park, PA (United States). Department of Chemical Engineering
  4. Univ. of Utah, Salt Lake City, UT (United States). Department of Chemistry
Publication Date:
Research Org.:
Univ. of Arkansas, Fayetteville, AR (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1481881
Grant/Contract Number:  
SC0016529
Resource Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 7; Journal ID: ISSN 2520-1158
Publisher:
Springer Nature
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Foster, Shelby L., Bakovic, Sergio I. Perez, Duda, Royce D., Maheshwari, Sharad, Milton, Ross D., Minteer, Shelley D., Janik, Michael J., Renner, Julie N., and Greenlee, Lauren F. Catalysts for nitrogen reduction to ammonia. United States: N. p., 2018. Web. doi:10.1038/s41929-018-0092-7.
Foster, Shelby L., Bakovic, Sergio I. Perez, Duda, Royce D., Maheshwari, Sharad, Milton, Ross D., Minteer, Shelley D., Janik, Michael J., Renner, Julie N., & Greenlee, Lauren F. Catalysts for nitrogen reduction to ammonia. United States. doi:https://doi.org/10.1038/s41929-018-0092-7
Foster, Shelby L., Bakovic, Sergio I. Perez, Duda, Royce D., Maheshwari, Sharad, Milton, Ross D., Minteer, Shelley D., Janik, Michael J., Renner, Julie N., and Greenlee, Lauren F. Thu . "Catalysts for nitrogen reduction to ammonia". United States. doi:https://doi.org/10.1038/s41929-018-0092-7. https://www.osti.gov/servlets/purl/1481881.
@article{osti_1481881,
title = {Catalysts for nitrogen reduction to ammonia},
author = {Foster, Shelby L. and Bakovic, Sergio I. Perez and Duda, Royce D. and Maheshwari, Sharad and Milton, Ross D. and Minteer, Shelley D. and Janik, Michael J. and Renner, Julie N. and Greenlee, Lauren F.},
abstractNote = {We present the production of synthetic ammonia remains dependent on the energy- and capital-intensive Haber-Bosch process. Extensive research in molecular catalysis has demonstrated ammonia production from di-nitrogen, albeit at low production rates. Mechanistic understanding of di-nitrogen reduction to ammonia continues to be delineated through study of molecular catalyst structure, as well as through understanding the naturally-occurring nitrogenase enzyme. The transition to Haber-Bosch alternatives through robust, heterogeneous catalyst surfaces remains an unsolved research challenge. Catalysts for electrochemical reduction of di-nitrogen to ammonia are a specific focus of research, due to the potential to compete with Haber-Bosch and eliminate associated carbon dioxide emissions. However, limited progress has been made, as most electrocatalyst surfaces lack specificity towards nitrogen fixation. Lastly in this review, we discuss the progress of the field in developing a mechanistic understanding of nitrogenase-promoted and molecular catalyst-promoted ammonia synthesis and provide a review of the state-of-the-art and scientific needs for heterogeneous electrocatalysts.},
doi = {10.1038/s41929-018-0092-7},
journal = {Nature Catalysis},
number = 7,
volume = 1,
place = {United States},
year = {2018},
month = {7}
}

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    Fe nanodot-decorated MoS 2 nanosheets on carbon cloth: an efficient and flexible electrode for ambient ammonia synthesis
    journal, January 2019

    • Zhao, Xinhui; Zhang, Xu; Xue, Zhimin
    • Journal of Materials Chemistry A, Vol. 7, Issue 48
    • DOI: 10.1039/c9ta09264a

    W supported on g-CN manifests high activity and selectivity for N 2 electroreduction to NH 3
    journal, January 2020

    • Wang, Shuhua; Wei, Wei; Lv, Xingshuai
    • Journal of Materials Chemistry A, Vol. 8, Issue 3
    • DOI: 10.1039/c9ta10935h

    Theory and experiments join forces to characterize the electrocatalytic interface
    journal, March 2019

    • Steinmann, Stephan N.; Wei, Zi-Yang; Sautet, Philippe
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 16
    • DOI: 10.1073/pnas.1903412116

    Complete cleavage of the N≡N triple bond by Ta 2 N + via degenerate ligand exchange at ambient temperature: A perfect catalytic cycle
    journal, October 2019

    • Geng, Caiyun; Li, Jilai; Weiske, Thomas
    • Proceedings of the National Academy of Sciences, Vol. 116, Issue 43
    • DOI: 10.1073/pnas.1913664116

    Investigating the operation parameters for ammonia synthesis in dielectric barrier discharge reactors
    journal, October 2019

    • Li, S.; van Raak, T.; Gallucci, F.
    • Journal of Physics D: Applied Physics, Vol. 53, Issue 1
    • DOI: 10.1088/1361-6463/ab4b37