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Chemical reviews
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7980-2020
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2020 v.120 no.12
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- Author:
- Devender Singh; William R. Buratto; Juan F. Torres; Leslie J. Murray
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5517-5581
- ISSN:
- 1520-6890
- Subject:
- actinides; ammonia; chemical bonding; ligands; metal ions; nitrogen; rare earth elements; surveys
- Abstract:
- ... Activation of dinitrogen plays an important role in daily anthropogenic life, and the processes by which this fixation occurs have been a longstanding and significant research focus within the community. One of the major fields of dinitrogen activation research is the use of multimetallic compounds to reduce and/or activate N₂ into a more useful nitrogen-atom source, such as ammonia. Here we repor ...
- DOI:
- 10.1021/acs.chemrev.0c00042
- https://doi.org/10.1021/acs.chemrev.0c00042
- Author:
- Sangmin Kim; Florian Loose; Paul J. Chirik
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5637-5681
- ISSN:
- 1520-6890
- Subject:
- Lewis acids; amines; ammonia; boron; carbon; catalysts; catalytic activity; chemical bonding; cycloaddition reactions; ligands; metals; nitrogen; nitrogen fixation; protonation; surveys; synthesis; thermodynamics
- Abstract:
- ... The functionalization of coordinated dinitrogen to form nitrogen–element bonds en route to nitrogen-containing molecules is a long-standing challenge in chemical synthesis. The strong triple bond and the nonpolarity of the N₂ molecule pose thermodynamic and kinetic challenges for promoting reactivity. While heterogeneous, homogeneous, and biological catalysts are all known for catalytic nitrogen f ...
- DOI:
- 10.1021/acs.chemrev.9b00705
- https://doi.org/10.1021/acs.chemrev.9b00705
- Author:
- Christina Ferousi; Sean H. Majer; Ida M. DiMucci; Kyle M. Lancaster
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5252-5307
- ISSN:
- 1520-6890
- Subject:
- chemical bonding; energy; fuels; hydrazine; lifestyle; metabolism; models; nitrogen; nitrous oxide
- Abstract:
- ... The metallobiochemistry underlying the formation of the inorganic N–N-bond-containing molecules nitrous oxide (N₂O), dinitrogen (N₂), and hydrazine (N₂H₄) is essential to the lifestyles of diverse organisms. Similar reactions hold promise as means to use N-based fuels as alternative carbon-free energy sources. This review discusses research efforts to understand the mechanisms underlying biologica ...
- DOI:
- 10.1021/acs.chemrev.9b00629
- https://doi.org/10.1021/acs.chemrev.9b00629
- Author:
- Stefan Burén; Emilio Jiménez-Vicente; Carlos Echavarri-Erasun; Luis M. Rubio
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 4921-4968
- ISSN:
- 1520-6890
- Subject:
- biosynthesis; iron; metallochaperones; nitrogenase
- Abstract:
- ... Nitrogenase harbors three distinct metal prosthetic groups that are required for its activity. The simplest one is a [4Fe-4S] cluster located at the Fe protein nitrogenase component. The MoFe protein component carries an [8Fe-7S] group called P-cluster and a [7Fe-9S-C-Mo-R-homocitrate] group called FeMo-co. Formation of nitrogenase metalloclusters requires the participation of the structural nitro ...
- DOI:
- 10.1021/acs.chemrev.9b00489
- https://doi.org/10.1021/acs.chemrev.9b00489
- Author:
- Kazuki Tanifuji; Yasuhiro Ohki
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5194-5251
- ISSN:
- 1520-6890
- Subject:
- ammonia; ligands; metals; nitrogen; nitrogen fixation; nitrogenase; prebiotics; sulfur
- Abstract:
- ... Transition metal–sulfur (M–S) compounds are an indispensable means for biological systems to convert N₂ into NH₃ (biological N₂ fixation), and these may have emerged by chemical evolution from a prebiotic N₂ fixation system. With a main focus on synthetic species, this article provides a comprehensive review of the chemistry of M–S compounds related to the conversion of N₂ and the structures/funct ...
- DOI:
- 10.1021/acs.chemrev.9b00544
- https://doi.org/10.1021/acs.chemrev.9b00544
- Author:
- Michael N. R. Ashfold; Jonathan P. Goss; Ben L. Green; Paul W. May; Mark E. Newton; Chloe V. Peaker
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5745-5794
- ISSN:
- 1520-6890
- Subject:
- annealing; hydrogen; nitrogen; surveys; temperature; vapors; world markets
- Abstract:
- ... Nitrogen is ubiquitous in both natural and laboratory-grown diamond, but the number and nature of the nitrogen-containing defects can have a profound effect on the diamond material and its properties. An ever-growing fraction of the supply of diamond appearing on the world market is now lab-grown. Here, we survey recent progress in two complementary diamond synthesis methods—high pressure high tem ...
- DOI:
- 10.1021/acs.chemrev.9b00518
- https://doi.org/10.1021/acs.chemrev.9b00518
- Author:
- Oren Elishav; Bar Mosevitzky Lis; Elisa M. Miller; Douglas J. Arent; Agustin Valera-Medina; Alon Grinberg Dana; Gennady E. Shter; Gideon S. Grader
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5352-5436
- ISSN:
- 1520-6890
- Subject:
- alternative fuels; ammonia; economic sustainability; energy; energy industry; environmental impact; fossil fuels; fuel combustion; infrastructure; nitrogen; renewable resources; synthetic fuels; turbines
- Abstract:
- ... Alternative fuels are essential to enable the transition to a sustainable and environmentally friendly energy supply. Synthetic fuels derived from renewable energies can act as energy storage media, thus mitigating the effects of fossil fuels on environment and health. Their economic viability, environmental impact, and compatibility with current infrastructure and technologies are fuel and power ...
- DOI:
- 10.1021/acs.chemrev.9b00538
- https://doi.org/10.1021/acs.chemrev.9b00538
- Author:
- Lance C. Seefeldt; Zhi-Yong Yang; Dmitriy A. Lukoyanov; Derek F. Harris; Dennis R. Dean; Simone Raugei; Brian M. Hoffman
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5082-5106
- ISSN:
- 1520-6890
- Subject:
- ammonia; carbon dioxide; carbon monoxide; catalysts; catalytic activity; enzyme substrates; fossil fuels; nitrogen; nitrogen fixation; nitrogenase
- Abstract:
- ... Nitrogenase is the enzyme that catalyzes biological N₂ reduction to NH₃. This enzyme achieves an impressive rate enhancement over the uncatalyzed reaction. Given the high demand for N₂ fixation to support food and chemical production and the heavy reliance of the industrial Haber–Bosch nitrogen fixation reaction on fossil fuels, there is a strong need to elucidate how nitrogenase achieves this dif ...
- DOI:
- 10.1021/acs.chemrev.9b00556
- https://doi.org/10.1021/acs.chemrev.9b00556
- Author:
- Matthew J. Chalkley; Marcus W. Drover; Jonas C. Peters
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5582-5636
- ISSN:
- 1520-6890
- Subject:
- ammonia; bioavailability; catalysts; catalytic activity; coordination compounds; enzymes; nitrogen; nitrogen fixation
- Abstract:
- ... Nitrogen fixation, the six-electron/six-proton reduction of N₂, to give NH₃, is one of the most challenging and important chemical transformations. Notwithstanding the barriers associated with this reaction, significant progress has been made in developing molecular complexes that reduce N₂ into its bioavailable form, NH₃. This progress is driven by the dual aims of better understanding biological ...
- DOI:
- 10.1021/acs.chemrev.9b00638
- https://doi.org/10.1021/acs.chemrev.9b00638
- Author:
- Hannah L. Rutledge; F. Akif Tezcan
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5158-5193
- ISSN:
- 1520-6890
- Subject:
- active sites; adenosine triphosphate; ammonia; catalytic activity; electrochemistry; electron transfer; electrons; energy; hydrolysis; nitrogen; nitrogenase; photochemistry; proteins; thermodynamics
- Abstract:
- ... Nitrogenase is the only enzyme capable of reducing N₂ to NH₃. This challenging reaction requires the coordinated transfer of multiple electrons from the reductase, Fe-protein, to the catalytic component, MoFe-protein, in an ATP-dependent fashion. In the last two decades, there have been significant advances in our understanding of how nitrogenase orchestrates electron transfer (ET) from the Fe-pro ...
- DOI:
- 10.1021/acs.chemrev.9b00663
- https://doi.org/10.1021/acs.chemrev.9b00663
11. Global Nitrogen Cycle: Critical Enzymes, Organisms, and Processes for Nitrogen Budgets and Dynamics
- Author:
- Xinning Zhang; Bess B. Ward; Daniel M. Sigman
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5308-5351
- ISSN:
- 1520-6890
- Subject:
- anthropogenic activities; biomass; carbon dioxide; enzymes; nitrogen; nitrogen cycle; nitrogen fixation
- Abstract:
- ... Nitrogen (N) is used in many of life’s fundamental biomolecules, and it is also a participant in environmental redox chemistry. Biogeochemical processes control the amount and form of N available to organisms (“fixed” N). These interacting processes result in N acting as the proximate limiting nutrient in most surface environments. Here, we review the global biogeochemical cycle of N and its anthr ...
- DOI:
- 10.1021/acs.chemrev.9b00613
- https://doi.org/10.1021/acs.chemrev.9b00613
- Author:
- Owen T. O’Sullivan; Michael J. Zdilla
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5682-5744
- ISSN:
- 1520-6890
- Subject:
- chemical bonding; chemical structure; explosives; nitrogen; nitrogen compounds; thermodynamics
- Abstract:
- ... The properties of catenated nitrogen molecules, molecules containing internal chains of bonded nitrogen atoms, is of fundamental scientific interest in chemical structure and bonding, as nitrogen is uniquely situated in the periodic table to form kinetically stable compounds often with chemically stable N–N bonds but which are thermodynamically unstable in that the formation of stable multiply bon ...
- DOI:
- 10.1021/acs.chemrev.9b00804
- https://doi.org/10.1021/acs.chemrev.9b00804
- Author:
- Andrew J. Jasniewski; Chi Chung Lee; Markus W. Ribbe; Yilin Hu
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5107-5157
- ISSN:
- 1520-6890
- Subject:
- biosynthesis; catalytic activity; chemical bonding; iron; multigene family; nitrogen; nitrogen fixation; nitrogenase; spectral analysis
- Abstract:
- ... Biological nitrogen fixation is catalyzed by the enzyme nitrogenase, which facilitates the cleavage of the relatively inert triple bond of N₂. Nitrogenase is most commonly associated with the molybdenum–iron cofactor called FeMoco or the M-cluster, and it has been the subject of extensive structural and spectroscopic characterization over the past 60 years. In the late 1980s and early 1990s, two “ ...
- DOI:
- 10.1021/acs.chemrev.9b00704
- https://doi.org/10.1021/acs.chemrev.9b00704
- Author:
- Geletu Qing; Reza Ghazfar; Shane T. Jackowski; Faezeh Habibzadeh; Mona Maleka Ashtiani; Chuan-Pin Chen; Milton R. Smith; Thomas W. Hamann
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5437-5516
- ISSN:
- 1520-6890
- Subject:
- ammonia; carbon dioxide; carbon footprint; catalytic activity; climate change; electrochemistry; electrolysis; gases; greenhouse gas emissions; hydrogen; hydrogen production; natural gas; nitrogen; nitrogen fixation; protons; renewable electricity; solar energy; temperature; wind power
- Abstract:
- ... Global ammonia production reached 175 million metric tons in 2016, 90% of which is produced from high purity N₂ and H₂ gases at high temperatures and pressures via the Haber–Bosch process. Reliance on natural gas for H₂ production results in large energy consumption and CO₂ emissions. Concerns of human-induced climate change are spurring an international scientific effort to explore new approaches ...
- DOI:
- 10.1021/acs.chemrev.9b00659
- https://doi.org/10.1021/acs.chemrev.9b00659
- Author:
- Casey Van Stappen; Laure Decamps; George E. Cutsail; Ragnar Bjornsson; Justin T. Henthorn; James A. Birrell; Serena DeBeer
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 5005-5081
- ISSN:
- 1520-6890
- Subject:
- active sites; enzymes; iron; models; molybdenum; nitrogen; nitrogen cycle; nitrogen fixation; spectral analysis; spectroscopy
- Abstract:
- ... Nitrogenases are responsible for biological nitrogen fixation, a crucial step in the biogeochemical nitrogen cycle. These enzymes utilize a two-component protein system and a series of iron–sulfur clusters to perform this reaction, culminating at the FeMco active site (M = Mo, V, Fe), which is capable of binding and reducing N₂ to 2NH₃. In this review, we summarize how different spectroscopic appr ...
- DOI:
- 10.1021/acs.chemrev.9b00650
- https://doi.org/10.1021/acs.chemrev.9b00650
- Author:
- Oliver Einsle; Douglas C. Rees
- Source:
- Chemical reviews 2020 v.120 no.12 pp. 4969-5004
- ISSN:
- 1520-6890
- Subject:
- active sites; ammonia; carbon; electrons; enzymology; hydrides; iron; ligands; models; nitrogen; nitrogenase; proteins; protons; reducing agents; spectroscopy
- Abstract:
- ... The reduction of dinitrogen to ammonia by nitrogenase reflects a complex choreography involving two component proteins, MgATP and reductant. At center stage of this process resides the active site cofactor, a complex metallocluster organized around a trigonal prismatic arrangement of iron sites surrounding an interstitial carbon. As a consequence of the choreography, electrons and protons are deli ...
- DOI:
- 10.1021/acs.chemrev.0c00067
- https://doi.org/10.1021/acs.chemrev.0c00067