Beyond fossil fuel–driven nitrogen transformations

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.

doi:10.1126/science.aar6611

Title: Beyond fossil fuel–driven nitrogen transformations

Journal Article · 24 May 2018 · Science

DOI: https://doi.org/10.1126/science.aar6611 · OSTI ID:1440394

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^[5]; Darensbourg, Marcetta Y. ^[6];

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^[8]; Janik, Michael J. ^[9];

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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)

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.

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Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1440394

Report Number(s):: NREL/JA--2700-70628

Journal Information:: Science, Journal Name: Science Journal Issue: 6391 Vol. 360; ISSN 0036-8075

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Crystal‐Phase‐Engineered PdCu Electrocatalyst for Enhanced Ammonia Synthesis Tong, Wu; Huang, Bolong; Wang, Pengtang Angewandte Chemie International Edition, Vol. 59, Issue 7 https://doi.org/10.1002/anie.201913122	journal	February 2020
The Crucial Role of Charge Accumulation and Spin Polarization in Activating Carbon‐Based Catalysts for Electrocatalytic Nitrogen Reduction Yang, Yuanyuan; Zhang, Lifu; Hu, Zhenpeng Angewandte Chemie International Edition, Vol. 59, Issue 11 https://doi.org/10.1002/anie.201915001	journal	February 2020
Transition‐Metal–Boron Intermetallics with Strong Interatomic d–sp Orbital Hybridization for High‐Performance Electrocatalysis Ai, Xuan; Zou, Xu; Chen, Hui Angewandte Chemie International Edition, Vol. 59, Issue 10 https://doi.org/10.1002/anie.201915663	journal	January 2020
Synergistic Promotion of the Electrochemical Reduction of Nitrogen to Ammonia by Phosphorus and Potassium Zhang, Qikun; Liu, Baoliang; Yu, Liping ChemCatChem, Vol. 12, Issue 1 https://doi.org/10.1002/cctc.201901519	journal	October 2019
A Combined Theory‐Experiment Analysis of the Surface Species in Lithium‐Mediated NH ₃ Electrosynthesis Schwalbe, Jay A.; Statt, Michael J.; Chosy, Cullen ChemElectroChem, Vol. 7, Issue 7 https://doi.org/10.1002/celc.201902124	journal	January 2020
A Combined Theory‐Experiment Analysis of the Surface Species in Lithium‐Mediated NH ₃ Electrosynthesis Schwalbe, Jay A.; Statt, Michael J.; Chosy, Cullen ChemElectroChem, Vol. 7, Issue 7 https://doi.org/10.1002/celc.202000265	journal	April 2020
Ambient Electrosynthesis of Ammonia on a Core–Shell‐Structured Au@CeO ₂ Catalyst: Contribution of Oxygen Vacancies in CeO ₂ Liu, Guoqiang; Cui, Zhiqing; Han, Miaomiao Chemistry – A European Journal, Vol. 25, Issue 23 https://doi.org/10.1002/chem.201806377	journal	March 2019
Advanced Non‐metallic Catalysts for Electrochemical Nitrogen Reduction under Ambient Conditions Zhang, Lili; Chen, Gao‐Feng; Ding, Liang‐Xin Chemistry – A European Journal, Vol. 25, Issue 54 https://doi.org/10.1002/chem.201901668	journal	July 2019
Ambient Electrochemical Synthesis of Ammonia from Nitrogen and Water Catalyzed by Flower-Like Gold Microstructures Wang, Ziqiang; Li, Yinghao; Yu, Hongjie ChemSusChem, Vol. 11, Issue 19 https://doi.org/10.1002/cssc.201801444	journal	September 2018
Fabrication of an Fe-Doped SrTiO ₃ Photocatalyst with Enhanced Dinitrogen Photofixation Performance: Fabrication of an Fe-Doped SrTiO ₃ Photocatalyst with Enhanced Dinitrogen Photofixation Performance Ying, Zihao; Chen, Shengtao; Peng, Tianyou European Journal of Inorganic Chemistry, Vol. 2019, Issue 16 https://doi.org/10.1002/ejic.201900098	journal	April 2019
Enhancement of Selective Fixation of Dinitrogen to Ammonia under Modal Strong Coupling Conditions: Enhancement of Selective Fixation of Dinitrogen to Ammonia under Modal Strong Coupling Conditions Oshikiri, Tomoya; Shi, Xu; Misawa, Hiroaki European Journal of Inorganic Chemistry, Vol. 2020, Issue 15-16 https://doi.org/10.1002/ejic.201901260	journal	February 2020
Enhancement of Selective Fixation of Dinitrogen to Ammonia under Modal Strong Coupling Conditions Oshikiri, Tomoya; Shi, Xu; Misawa, Hiroaki European Journal of Inorganic Chemistry, Vol. 2020, Issue 15-16 https://doi.org/10.1002/ejic.202000340	journal	April 2020
Electrochemical Fabrication of Porous Au Film on Ni Foam for Nitrogen Reduction to Ammonia Wang, Hongjing; Yu, Hongjie; Wang, Ziqiang Small, Vol. 15, Issue 6 https://doi.org/10.1002/smll.201804769	journal	January 2019
Defect Engineering Strategies for Nitrogen Reduction Reactions under Ambient Conditions Yan, Dafeng; Li, Hao; Chen, Chen Small Methods, Vol. 3, Issue 6 https://doi.org/10.1002/smtd.201800331	journal	October 2018
Computational Screening of Efficient Single‐Atom Catalysts Based on Graphitic Carbon Nitride (g‐C ₃ N ₄ ) for Nitrogen Electroreduction Chen, Zhe; Zhao, Jingxiang; Cabrera, Carlos R. Small Methods, Vol. 3, Issue 6 https://doi.org/10.1002/smtd.201800368	journal	October 2018
Recent Progress on Electrocatalyst and Photocatalyst Design for Nitrogen Reduction Li, Mengqiao; Huang, Hao; Low, Jingxiang Small Methods, Vol. 3, Issue 6 https://doi.org/10.1002/smtd.201800388	journal	October 2018
Is It Appropriate to Use the Nafion Membrane in Electrocatalytic N ₂ Reduction? Ren, Yongwen; Yu, Chang; Tan, Xinyi Small Methods, Vol. 3, Issue 12 https://doi.org/10.1002/smtd.201900474	journal	August 2019
Advances and challenges in modeling solvated reaction mechanisms for renewable fuels and chemicals Basdogan, Yasemin; Maldonado, Alex M.; Keith, John A. WIREs Computational Molecular Science, Vol. 10, Issue 2 https://doi.org/10.1002/wcms.1446	journal	August 2019
3D Hierarchical Porous Graphene-Based Energy Materials: Synthesis, Functionalization, and Application in Energy Storage and Conversion Tang, Cheng; Wang, Hao-Fan; Huang, Jia-Qi Electrochemical Energy Reviews, Vol. 2, Issue 2 https://doi.org/10.1007/s41918-019-00033-7	journal	March 2019
Facilitating nitrogen accessibility to boron-rich covalent organic frameworks via electrochemical excitation for efficient nitrogen fixation Liu, Sisi; Wang, Mengfan; Qian, Tao Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-11846-x	journal	August 2019
Formation of carbon–nitrogen bonds in carbon monoxide electrolysis Jouny, Matthew; Lv, Jing-Jing; Cheng, Tao Nature Chemistry, Vol. 11, Issue 9 https://doi.org/10.1038/s41557-019-0312-z	journal	August 2019
Capture of nitrogen dioxide and conversion to nitric acid in a porous metal–organic framework Li, Jiangnan; Han, Xue; Zhang, Xinran Nature Chemistry, Vol. 11, Issue 12 https://doi.org/10.1038/s41557-019-0356-0	journal	November 2019
The technological and economic prospects for CO2 utilization and removal Hepburn, Cameron; Adlen, Ella; Beddington, John Nature, Vol. 575, Issue 7781 https://doi.org/10.1038/s41586-019-1681-6	journal	November 2019
Promoting nitrogen electroreduction to ammonia with bismuth nanocrystals and potassium cations in water Hao, Yu-Chen; Guo, Yu; Chen, Li-Wei Nature Catalysis, Vol. 2, Issue 5 https://doi.org/10.1038/s41929-019-0241-7	journal	March 2019
Electrochemical nitrogen reduction to ammonia at ambient conditions on nitrogen and phosphorus co-doped porous carbon Song, Pengfei; Wang, Hao; Kang, Li Chemical Communications, Vol. 55, Issue 5 https://doi.org/10.1039/c8cc09256g	journal	January 2019
One-pot synthesis of bi-metallic PdRu tripods as an efficient catalyst for electrocatalytic nitrogen reduction to ammonia Wang, Hongjing; Li, Yinghao; Li, Chunjie Journal of Materials Chemistry A, Vol. 7, Issue 2 https://doi.org/10.1039/c8ta09482a	journal	January 2019
Trimetallic PdCuIr with long-spined sea-urchin-like morphology for ambient electroreduction of nitrogen to ammonia Kumar, Rajaiah Dhilip; Wang, Ziqiang; Li, Chunjie Journal of Materials Chemistry A, Vol. 7, Issue 7 https://doi.org/10.1039/c8ta10562f	journal	January 2019
Cu doping in CeO ₂ to form multiple oxygen vacancies for dramatically enhanced ambient N ₂ reduction performance Zhang, Shengbo; Zhao, Cuijiao; Liu, Yanyan Chemical Communications, Vol. 55, Issue 20 https://doi.org/10.1039/c9cc00123a	journal	January 2019
B ₄ C nanosheets decorated with in situ -derived boron-doped graphene quantum dots for high-efficiency ambient N ₂ fixation Qiu, Wei-Bin; Luo, Yu-Xi; Liang, Ru-Ping Chemical Communications, Vol. 55, Issue 51 https://doi.org/10.1039/c9cc03413g	journal	January 2019
Morphology-dependent electrocatalytic nitrogen reduction on Ag triangular nanoplates Gao, Wen-Yan; Hao, Yu-Chen; Su, Xin Chemical Communications, Vol. 55, Issue 72 https://doi.org/10.1039/c9cc04691g	journal	January 2019
Synthesis of ammonia via electrochemical nitrogen reduction on high-index faceted Au nanoparticles with a high faradaic efficiency Tan, Lianqiao; Yang, Na; Huang, Xun Chemical Communications, Vol. 55, Issue 96 https://doi.org/10.1039/c9cc06132k	journal	January 2019
High-efficiency electrocatalyst for N ₂ conversion to NH ₃ based on Au nanoparticles loaded on defective WO _3−x Li, Youzeng; Yan, Pengfei; Chen, Jun Chemical Communications, Vol. 55, Issue 88 https://doi.org/10.1039/c9cc06550d	journal	January 2019
Triple hydrogen atom abstraction from Mn–NH 3 complexes results in cyclophosphazenium cations Cook, Brian J.; Johnson, Samantha I.; Chambers, Geoffrey M. Chemical Communications, Vol. 55, Issue 93 https://doi.org/10.1039/c9cc06915a	journal	January 2019
Tuning the catalytic activity of a single Mo atom supported on graphene for nitrogen reduction via Se atom doping Zhou, Hong Yu; Li, Jian Chen; Wen, Zi Physical Chemistry Chemical Physics, Vol. 21, Issue 27 https://doi.org/10.1039/c9cp02733e	journal	January 2019
Understanding electro-catalysis by using density functional theory Chen, Z. W.; Chen, L. X.; Wen, Z. Physical Chemistry Chemical Physics, Vol. 21, Issue 43 https://doi.org/10.1039/c9cp04430b	journal	January 2019
Electrochemical nitrogen fixation and utilization: theories, advanced catalyst materials and system design Guo, Wenhan; Zhang, Kexin; Liang, Zibin Chemical Society Reviews, Vol. 48, Issue 24 https://doi.org/10.1039/c9cs00159j	journal	January 2019
How to explore ambient electrocatalytic nitrogen reduction reliably and insightfully Tang, Cheng; Qiao, Shi-Zhang Chemical Society Reviews, Vol. 48, Issue 12 https://doi.org/10.1039/c9cs00280d	journal	January 2019
Chemical looping beyond combustion – a perspective Zhu, Xing; Imtiaz, Qasim; Donat, Felix Energy & Environmental Science, Vol. 13, Issue 3 https://doi.org/10.1039/c9ee03793d	journal	January 2020
Anion (O, N, C, and S) vacancies promoted photocatalytic nitrogen fixation Mao, Chengliang; Wang, Jiaxian; Zou, Yunjie Green Chemistry, Vol. 21, Issue 11 https://doi.org/10.1039/c9gc01010f	journal	January 2019
Single molybdenum center supported on N-doped black phosphorus as an efficient electrocatalyst for nitrogen fixation Ou, Pengfei; Zhou, Xiao; Meng, Fanchao Nanoscale, Vol. 11, Issue 28 https://doi.org/10.1039/c9nr02586c	journal	January 2019
Selective decontamination of the reactive air pollutant nitrous acid via node-linker cooperativity in a metal–organic framework McGrath, Devon T.; Ryan, Michaela D.; MacInnis, John J. Chemical Science, Vol. 10, Issue 21 https://doi.org/10.1039/c9sc01357a	journal	January 2019
Excitonic Au ₄ Ru ₂ (PPh ₃ ) ₂ (SC ₂ H ₄ Ph) ₈ cluster for light-driven dinitrogen fixation Sun, Yongnan; Pei, Wei; Xie, Mingcai Chemical Science, Vol. 11, Issue 9 https://doi.org/10.1039/c9sc06424a	journal	January 2020
Pt-embedded in monolayer g-C ₃ N ₄ as a promising single-atom electrocatalyst for ammonia synthesis Yin, Hui; Li, Shu-Long; Gan, Li-Yong Journal of Materials Chemistry A, Vol. 7, Issue 19 https://doi.org/10.1039/c9ta01624d	journal	January 2019
Fluorine-free Ti ₃ C ₂ T _x (T = O, OH) nanosheets (∼50–100 nm) for nitrogen fixation under ambient conditions Li, Tengfei; Yan, Xudong; Huang, Lujun Journal of Materials Chemistry A, Vol. 7, Issue 24 https://doi.org/10.1039/c9ta03254a	journal	January 2019
Bimetallic Ag ₃ Cu porous networks for ambient electrolysis of nitrogen to ammonia Yu, Hongjie; Wang, Ziqiang; Yang, Dandan Journal of Materials Chemistry A, Vol. 7, Issue 20 https://doi.org/10.1039/c9ta03297e	journal	January 2019
Electron distribution tuning of fluorine-doped carbon for ammonia electrosynthesis Yuan, Di; Wei, Zengxi; Han, Peng Journal of Materials Chemistry A, Vol. 7, Issue 28 https://doi.org/10.1039/c9ta04141a	journal	January 2019
Facile, cost-effective plasma synthesis of self-supportive FeS _x on Fe foam for efficient electrochemical reduction of N ₂ under ambient conditions Xiong, Wei; Guo, Zheng; Zhao, Shijun Journal of Materials Chemistry A, Vol. 7, Issue 34 https://doi.org/10.1039/c9ta07790a	journal	January 2019
Atomically dispersed metal dimer species with selective catalytic activity for nitrogen electrochemical reduction Li, Yang; Zhang, Qi; Li, Can Journal of Materials Chemistry A, Vol. 7, Issue 39 https://doi.org/10.1039/c9ta07845b	journal	January 2019
Theoretical insights into nonprecious oxygen-evolution active sites in Ti–Ir-Based perovskite solid solution electrocatalysts Shi, Lei; Chen, Hui; Liang, Xiao Journal of Materials Chemistry A, Vol. 8, Issue 1 https://doi.org/10.1039/c9ta10059h	journal	January 2020
W supported on g-CN manifests high activity and selectivity for N ₂ electroreduction to NH ₃ Wang, Shuhua; Wei, Wei; Lv, Xingshuai Journal of Materials Chemistry A, Vol. 8, Issue 3 https://doi.org/10.1039/c9ta10935h	journal	January 2020
Complete cleavage of the N≡N triple bond by Ta ₂ N ⁺ via degenerate ligand exchange at ambient temperature: A perfect catalytic cycle Geng, Caiyun; Li, Jilai; Weiske, Thomas Proceedings of the National Academy of Sciences, Vol. 116, Issue 43 https://doi.org/10.1073/pnas.1913664116	journal	October 2019
Specific energy cost for nitrogen fixation as NO _x using DC glow discharge in air Pei, Xuekai; Gidon, Dogan; Graves, David B. Journal of Physics D: Applied Physics, Vol. 53, Issue 4 https://doi.org/10.1088/1361-6463/ab5095	journal	November 2019
Electrochemical synthesis of nitric acid from air and ammonia through waste utilization Wang, Yuting; Yu, Yifu; Jia, Ranran National Science Review, Vol. 6, Issue 4 https://doi.org/10.1093/nsr/nwz019	journal	February 2019
Dissociating stable nitrogen molecules under mild conditions by cyclic strain engineering Han, Gao-Feng; Shi, Xiang-Mei; Kim, Seok-Jin Science Advances, Vol. 5, Issue 11 https://doi.org/10.1126/sciadv.aax8275	journal	November 2019
Visible-Light Bismuth Iron Molybdate Photocatalyst for Artificial Nitrogen Fixation Liu, Botong; Yasin, Alhassan S.; Musho, Terrence Journal of The Electrochemical Society, Vol. 166, Issue 5 https://doi.org/10.1149/2.0151905jes	journal	January 2019
Selective Electrochemical Reduction of Nitrogen to Ammonia by Adjusting the Three-Phase Interface Wang, Haiyan; Chen, Yuzhuo; Fan, Ruxue Research, Vol. 2019 https://doi.org/10.34133/2019/1401209	journal	November 2019

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