Beyond fossil fuel–driven nitrogen transformations
Abstract
Nitrogen is fundamental to all of life and many industrial processes. The interchange of nitrogen oxidation states in the industrial production of ammonia, nitric acid, and other commodity chemicals is largely powered by fossil fuels. Here, a key goal of contemporary research in the field of nitrogen chemistry is to minimize the use of fossil fuels by developing more efficient heterogeneous, homogeneous, photo-, and electrocatalytic processes or by adapting the enzymatic processes underlying the natural nitrogen cycle. These approaches, as well as the challenges involved, are discussed in this Review.
- Authors:
-
- Columbia Univ., New York, NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
- The Univ. of Texas at Austin, Austin, TX (United States)
- Utah State Univ., Logan, UT (United States)
- Univ. of Rochester, Rochester, NY (United States)
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Texas A & M Univ., College Station, TX (United States)
- Yale Univ., New Haven, CT (United States)
- Northwestern Univ., Evanston, IL (United States)
- Pennsylvania State Univ., University Park, PA (United States)
- Arizona State Univ., Tempe, AZ (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Cornell Univ., Ithaca, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Washington State Univ., Pullman, WA (United States)
- Univ. of Notre Dame, Notre Dame, IN (United States)
- Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1440394
- Report Number(s):
- NREL/JA-2700-70628
Journal ID: ISSN 0036-8075
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Science
- Additional Journal Information:
- Journal Volume: 360; Journal Issue: 6391; Journal ID: ISSN 0036-8075
- Publisher:
- AAAS
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 09 BIOMASS FUELS; nitrogen; fossil fuels; chemistry
Citation Formats
Chen, Jingguang G., Crooks, Richard M., Seefeldt, Lance C., Bren, Kara L., Bullock, R. Morris, Darensbourg, Marcetta Y., Holland, Patrick L., Hoffman, Brian, Janik, Michael J., Jones, Anne K., Kanatzidis, Mercouri G., King, Paul, Lancaster, Kyle M., Lymar, Sergei V., Pfromm, Peter, Schneider, William F., and Schrock, Richard R.. Beyond fossil fuel–driven nitrogen transformations. United States: N. p., 2018.
Web. doi:10.1126/science.aar6611.
Chen, Jingguang G., Crooks, Richard M., Seefeldt, Lance C., Bren, Kara L., Bullock, R. Morris, Darensbourg, Marcetta Y., Holland, Patrick L., Hoffman, Brian, Janik, Michael J., Jones, Anne K., Kanatzidis, Mercouri G., King, Paul, Lancaster, Kyle M., Lymar, Sergei V., Pfromm, Peter, Schneider, William F., & Schrock, Richard R.. Beyond fossil fuel–driven nitrogen transformations. United States. https://doi.org/10.1126/science.aar6611
Chen, Jingguang G., Crooks, Richard M., Seefeldt, Lance C., Bren, Kara L., Bullock, R. Morris, Darensbourg, Marcetta Y., Holland, Patrick L., Hoffman, Brian, Janik, Michael J., Jones, Anne K., Kanatzidis, Mercouri G., King, Paul, Lancaster, Kyle M., Lymar, Sergei V., Pfromm, Peter, Schneider, William F., and Schrock, Richard R.. Fri .
"Beyond fossil fuel–driven nitrogen transformations". United States. https://doi.org/10.1126/science.aar6611. https://www.osti.gov/servlets/purl/1440394.
@article{osti_1440394,
title = {Beyond fossil fuel–driven nitrogen transformations},
author = {Chen, Jingguang G. and Crooks, Richard M. and Seefeldt, Lance C. and Bren, Kara L. and Bullock, R. Morris and Darensbourg, Marcetta Y. and Holland, Patrick L. and Hoffman, Brian and Janik, Michael J. and Jones, Anne K. and Kanatzidis, Mercouri G. and King, Paul and Lancaster, Kyle M. and Lymar, Sergei V. and Pfromm, Peter and Schneider, William F. and Schrock, Richard R.},
abstractNote = {Nitrogen is fundamental to all of life and many industrial processes. The interchange of nitrogen oxidation states in the industrial production of ammonia, nitric acid, and other commodity chemicals is largely powered by fossil fuels. Here, a key goal of contemporary research in the field of nitrogen chemistry is to minimize the use of fossil fuels by developing more efficient heterogeneous, homogeneous, photo-, and electrocatalytic processes or by adapting the enzymatic processes underlying the natural nitrogen cycle. These approaches, as well as the challenges involved, are discussed in this Review.},
doi = {10.1126/science.aar6611},
journal = {Science},
number = 6391,
volume = 360,
place = {United States},
year = {Fri May 25 00:00:00 EDT 2018},
month = {Fri May 25 00:00:00 EDT 2018}
}
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Figures / Tables:
Figure 1: Atom and energy economy of nitrogen fixation. The numerical values represent standard (14) Gibbs free energies in kJ/mol of fixed $N$2 in the direction of the arrows. All thermochemical data are from (15), except for H2NOH.
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Synthesis of ammonia via electrochemical nitrogen reduction on high-index faceted Au nanoparticles with a high faradaic efficiency
journal, January 2019
- Tan, Lianqiao; Yang, Na; Huang, Xun
- Chemical Communications, Vol. 55, Issue 96
High-efficiency electrocatalyst for N 2 conversion to NH 3 based on Au nanoparticles loaded on defective WO 3−x
journal, January 2019
- Li, Youzeng; Yan, Pengfei; Chen, Jun
- Chemical Communications, Vol. 55, Issue 88
Triple hydrogen atom abstraction from Mn–NH 3 complexes results in cyclophosphazenium cations
journal, January 2019
- Cook, Brian J.; Johnson, Samantha I.; Chambers, Geoffrey M.
- Chemical Communications, Vol. 55, Issue 93
How to explore ambient electrocatalytic nitrogen reduction reliably and insightfully
journal, January 2019
- Tang, Cheng; Qiao, Shi-Zhang
- Chemical Society Reviews, Vol. 48, Issue 12
Chemical looping beyond combustion – a perspective
journal, January 2020
- Zhu, Xing; Imtiaz, Qasim; Donat, Felix
- Energy & Environmental Science, Vol. 13, Issue 3
Anion (O, N, C, and S) vacancies promoted photocatalytic nitrogen fixation
journal, January 2019
- Mao, Chengliang; Wang, Jiaxian; Zou, Yunjie
- Green Chemistry, Vol. 21, Issue 11
Single molybdenum center supported on N-doped black phosphorus as an efficient electrocatalyst for nitrogen fixation
journal, January 2019
- Ou, Pengfei; Zhou, Xiao; Meng, Fanchao
- Nanoscale, Vol. 11, Issue 28
Excitonic Au 4 Ru 2 (PPh 3 ) 2 (SC 2 H 4 Ph) 8 cluster for light-driven dinitrogen fixation
journal, January 2020
- Sun, Yongnan; Pei, Wei; Xie, Mingcai
- Chemical Science, Vol. 11, Issue 9
Bimetallic Ag 3 Cu porous networks for ambient electrolysis of nitrogen to ammonia
journal, January 2019
- Yu, Hongjie; Wang, Ziqiang; Yang, Dandan
- Journal of Materials Chemistry A, Vol. 7, Issue 20
Theoretical insights into nonprecious oxygen-evolution active sites in Ti–Ir-Based perovskite solid solution electrocatalysts
journal, January 2020
- Shi, Lei; Chen, Hui; Liang, Xiao
- Journal of Materials Chemistry A, Vol. 8, Issue 1
Electrochemical synthesis of nitric acid from air and ammonia through waste utilization
journal, February 2019
- Wang, Yuting; Yu, Yifu; Jia, Ranran
- National Science Review, Vol. 6, Issue 4
Dissociating stable nitrogen molecules under mild conditions by cyclic strain engineering
journal, November 2019
- Han, Gao-Feng; Shi, Xiang-Mei; Kim, Seok-Jin
- Science Advances, Vol. 5, Issue 11
Visible-Light Bismuth Iron Molybdate Photocatalyst for Artificial Nitrogen Fixation
journal, January 2019
- Liu, Botong; Yasin, Alhassan S.; Musho, Terrence
- Journal of The Electrochemical Society, Vol. 166, Issue 5
Selective Electrochemical Reduction of Nitrogen to Ammonia by Adjusting the Three-Phase Interface
journal, November 2019
- Wang, Haiyan; Chen, Yuzhuo; Fan, Ruxue
- Research, Vol. 2019
Nitrogen Vacancies on 2D Layered W 2 N 3 : A Stable and Efficient Active Site for Nitrogen Reduction Reaction
journal, June 2019
- Jin, Huanyu; Li, Laiquan; Liu, Xin
- Advanced Materials
A General Strategy to Glassy M‐Te (M = Ru, Rh, Ir) Porous Nanorods for Efficient Electrochemical N 2 Fixation
journal, February 2020
- Wang, Juan; Huang, Bolong; Ji, Yujin
- Advanced Materials, Vol. 32, Issue 11
Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction
journal, January 2020
- Huang, Yiyin; Babu, Dickson D.; Peng, Zhen
- Advanced Science, Vol. 7, Issue 4
Aryldiazonium Salts as Nitrogen-Based Lewis Acids: Facile Synthesis of Tuneable Azophosphonium Salts
journal, August 2018
- Habraken, Evi R. M.; van Leest, Nicolaas P.; Hooijschuur, Pim
- Angewandte Chemie, Vol. 130, Issue 37
A Combined Theory‐Experiment Analysis of the Surface Species in Lithium‐Mediated NH 3 Electrosynthesis
journal, January 2020
- Schwalbe, Jay A.; Statt, Michael J.; Chosy, Cullen
- ChemElectroChem, Vol. 7, Issue 7
Formation of carbon–nitrogen bonds in carbon monoxide electrolysis
journal, August 2019
- Jouny, Matthew; Lv, Jing-Jing; Cheng, Tao
- Nature Chemistry, Vol. 11, Issue 9
One-pot synthesis of bi-metallic PdRu tripods as an efficient catalyst for electrocatalytic nitrogen reduction to ammonia
journal, January 2019
- Wang, Hongjing; Li, Yinghao; Li, Chunjie
- Journal of Materials Chemistry A, Vol. 7, Issue 2
B 4 C nanosheets decorated with in situ -derived boron-doped graphene quantum dots for high-efficiency ambient N 2 fixation
journal, January 2019
- Qiu, Wei-Bin; Luo, Yu-Xi; Liang, Ru-Ping
- Chemical Communications, Vol. 55, Issue 51
Morphology-dependent electrocatalytic nitrogen reduction on Ag triangular nanoplates
journal, January 2019
- Gao, Wen-Yan; Hao, Yu-Chen; Su, Xin
- Chemical Communications, Vol. 55, Issue 72
Tuning the catalytic activity of a single Mo atom supported on graphene for nitrogen reduction via Se atom doping
journal, January 2019
- Zhou, Hong Yu; Li, Jian Chen; Wen, Zi
- Physical Chemistry Chemical Physics, Vol. 21, Issue 27
Understanding electro-catalysis by using density functional theory
journal, January 2019
- Chen, Z. W.; Chen, L. X.; Wen, Z.
- Physical Chemistry Chemical Physics, Vol. 21, Issue 43
Selective decontamination of the reactive air pollutant nitrous acid via node-linker cooperativity in a metal–organic framework
journal, January 2019
- McGrath, Devon T.; Ryan, Michaela D.; MacInnis, John J.
- Chemical Science, Vol. 10, Issue 21
Electron distribution tuning of fluorine-doped carbon for ammonia electrosynthesis
journal, January 2019
- Yuan, Di; Wei, Zengxi; Han, Peng
- Journal of Materials Chemistry A, Vol. 7, Issue 28
Facile, cost-effective plasma synthesis of self-supportive FeS x on Fe foam for efficient electrochemical reduction of N 2 under ambient conditions
journal, January 2019
- Xiong, Wei; Guo, Zheng; Zhao, Shijun
- Journal of Materials Chemistry A, Vol. 7, Issue 34
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
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
Specific energy cost for nitrogen fixation as NO x using DC glow discharge in air
journal, November 2019
- Pei, Xuekai; Gidon, Dogan; Graves, David B.
- Journal of Physics D: Applied Physics, Vol. 53, Issue 4
Molybdenum Carbide Nanodots Enable Efficient Electrocatalytic Nitrogen Fixation under Ambient Conditions
journal, October 2018
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- Advanced Materials, Vol. 30, Issue 46
High Efficiency Electrochemical Nitrogen Fixation Achieved with a Lower Pressure Reaction System by Changing the Chemical Equilibrium
journal, September 2019
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A Combined Theory‐Experiment Analysis of the Surface Species in Lithium‐Mediated NH 3 Electrosynthesis
journal, April 2020
- Schwalbe, Jay A.; Statt, Michael J.; Chosy, Cullen
- ChemElectroChem, Vol. 7, Issue 7
Advanced Non‐metallic Catalysts for Electrochemical Nitrogen Reduction under Ambient Conditions
journal, July 2019
- Zhang, Lili; Chen, Gao‐Feng; Ding, Liang‐Xin
- Chemistry – A European Journal, Vol. 25, Issue 54
Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation
journal, August 2019
- Liu, Sisi; Wang, Mengfan; Qian, Tao
- Nature Communications, Vol. 10, Issue 1
Electrochemical nitrogen fixation and utilization: theories, advanced catalyst materials and system design
journal, January 2019
- Guo, Wenhan; Zhang, Kexin; Liang, Zibin
- Chemical Society Reviews, Vol. 48, Issue 24
Pt-embedded in monolayer g-C 3 N 4 as a promising single-atom electrocatalyst for ammonia synthesis
journal, January 2019
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- Journal of Materials Chemistry A, Vol. 7, Issue 19
Atomically dispersed metal dimer species with selective catalytic activity for nitrogen electrochemical reduction
journal, January 2019
- Li, Yang; Zhang, Qi; Li, Can
- Journal of Materials Chemistry A, Vol. 7, Issue 39
Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation
journal, January 2019
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- Angewandte Chemie, Vol. 131, Issue 8
Enhancement of Selective Fixation of Dinitrogen to Ammonia under Modal Strong Coupling Conditions
journal, April 2020
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- European Journal of Inorganic Chemistry, Vol. 2020, Issue 15-16
Ammonia Synthesis Under Ambient Conditions: Selective Electroreduction of Dinitrogen to Ammonia on Black Phosphorus Nanosheets
journal, January 2019
- Zhang, Lili; Ding, Liang‐Xin; Chen, Gao‐Feng
- Angewandte Chemie, Vol. 131, Issue 9
Catalytic Ammonia Oxidation to Dinitrogen by Hydrogen Atom Abstraction
journal, June 2019
- Bhattacharya, Papri; Heiden, Zachariah M.; Chambers, Geoffrey M.
- Angewandte Chemie International Edition, Vol. 58, Issue 34
Fluorine-free Ti 3 C 2 T x (T = O, OH) nanosheets (∼50–100 nm) for nitrogen fixation under ambient conditions
journal, January 2019
- Li, Tengfei; Yan, Xudong; Huang, Lujun
- Journal of Materials Chemistry A, Vol. 7, Issue 24
Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction
journal, January 2020
- Huang, Yiyin; Babu, Dickson D.; Peng, Zhen
- Advanced Science, Vol. 7, Issue 4
Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation
journal, August 2019
- Liu, Sisi; Wang, Mengfan; Qian, Tao
- Nature Communications, Vol. 10, Issue 1
Steric Switching From Photochemical to Thermal N2 Splitting: A Computational Analysis of the Isomerization Reaction {(Cp*)(Am)Mo}2(μ-η1:η1-N2) → {(Cp*)(Am)Mo}2(μ-N)2
journal, May 2019
- Krewald, Vera
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Omeprazole Treatment Enhances Nitrogen Use Efficiency Through Increased Nitrogen Uptake and Assimilation in Corn
journal, December 2019
- Van Oosten, Michael James; Dell’Aversana, Emilia; Ruggiero, Alessandra
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Selective Electrochemical Reduction of Nitrogen to Ammonia by Adjusting the Three-Phase Interface
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