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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. 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.

SUBMITTER: Chen JG

PROVIDER: S-EPMC6088796 | biostudies-literature | 2018 May

REPOSITORIES: biostudies-literature

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Beyond fossil fuel-driven nitrogen transformations.

Chen Jingguang G JG Crooks Richard M RM Seefeldt Lance C LC Bren Kara L KL Bullock R Morris RM Darensbourg Marcetta Y MY Holland Patrick L PL Hoffman Brian B Janik Michael J MJ Jones Anne K AK Kanatzidis Mercouri G MG King Paul P Lancaster Kyle M KM Lymar Sergei V SV Pfromm Peter P Schneider William F WF Schrock Richard R RR

Science (New York, N.Y.) 20180501 6391

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. 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 natur ...[more]

PMID: 29798857

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Project description:Vegetation fires are known to have broad geochemical effects on carbon (C) cycles in the Earth system, yet limited information is available for nitrogen (N). In this study, we evaluated how charring organic matter (OM) to pyrogenic OM (PyOM) altered the N molecular structure and affected subsequent C and N mineralization. Nitrogen near-edge X-ray absorption fine structure (NEXAFS) of uncharred OM, PyOM, PyOM toluene extract, and PyOM after toluene extraction were used to predict PyOM-C and -N mineralization potentials. PyOM was produced from three different plants (e.g. Maize-Zea mays L.; Ryegrass-Lollium perenne L.; and Willow-Salix viminalix L.) each with varying initial N contents at three pyrolysis temperatures (350, 500 and 700?°C). Mineralization of C and N was measured from incubations of uncharred OM and PyOM in a sand matrix for 256?days at 30?°C. As pyrolysis temperature increased from 350 to 700?°C, aromatic C[bond, double bond]N in 6-membered rings (putative) increased threefold. Aromatic C[bond, double bond]N in 6-membered oxygenated ring increased sevenfold, and quaternary aromatic N doubled. Initial uncharred OM-N content was positively correlated with the proportion of heterocyclic aromatic N in PyOM (R2?=?0.44; P?<?0.0001; n?=?42). A 55% increase of aromatic N heterocycles at high OM-N content, when compared to low OM-N content, suggests that higher concentrations of N favor the incorporation of N atoms into aromatic structures by overcoming the energy barrier associated with the electronic and atomic configuration of the C structure. A ten-fold increase of aromatic C[bond, double bond]N in 6-membered rings (putative) in PyOM (as proportion of all PyOM-N) decreased C mineralization by 87%, whereas total N contents and C:N ratios of PyOM had no effects on C mineralization of PyOM-C for both pyrolysis temperatures (for PyOM-350?°C, R2?=?0.15; P?<?0.27; for PyOM-700?°C, R2?=?0.22; P?<?0.21). Oxidized aromatic N in PyOM toluene extracts correlated with higher C mineralization, whereas aromatic N in 6-membered heterocycles correlated with reduced C mineralization (R2?=?0.56; P?=?0.001; n?=?100). Similarly, aromatic N in 6-membered heterocycles in PyOM remaining after toluene extraction reduced PyOM-C mineralization (R2?=?0.49; P?=?0.0006; n?=?100). PyOM-C mineralization increased when N atoms were located at the edge of the C network in the form of oxidized N functionalities or when more N was found in PyOM toluene extracts and was more accessible to microbial oxidation. These results confirm the hypothesis that C persistence of fire-derived OM is significantly affected by its molecular N structure and the presented quantitative structure-activity relationship can be utilized for predictive modeling purposes.

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Beyond fossil fuel-driven nitrogen transformations.

Publications

Beyond fossil fuel-driven nitrogen transformations.

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