Lignin-enhanced reduction of structural Fe(III) in nontronite: Dual roles of lignin as electron shuttle and donor

Sheng, Yizhi; Dong, Hailiang; Kukkadapu, Ravi K.; Ni, Shuisong; Zeng, Qiang; Hu, Jinglong; Coffin, Ethan; Zhao, Simin; Sommer, Andre J.; McCarrick, Robert M.; Lorigan, Gary A.

doi:10.1016/j.gca.2021.05.037

Title: Lignin-enhanced reduction of structural Fe(III) in nontronite: Dual roles of lignin as electron shuttle and donor

Journal Article · Wed May 26 00:00:00 EDT 2021 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2021.05.037· OSTI ID:1812535

Sheng, Yizhi ^[1]; Dong, Hailiang ^[2];

^[3]; Ni, Shuisong ^[4]; Zeng, Qiang ^[5]; Hu, Jinglong ^[5]; Coffin, Ethan ^[1]; Zhao, Simin ^[1]; Sommer, Andre J. ^[4];

^[4]; Lorigan, Gary A. ^[4]

Miami Univ., Oxford, OH (United States). Dept. of Geology and Environmental Earth Science
Miami Univ., Oxford, OH (United States). Dept. of Geology and Environmental Earth Science; China Univ. of Geosciences, Beijing (China). State Key Laboratory of Biogeology and Environmental Geology
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Miami Univ., Oxford, OH (United States). Dept. of Chemistry and Biochemistry
China Univ. of Geosciences, Beijing (China). State Key Laboratory of Biogeology and Environmental Geology

Lignin is a major component of plant-derived soil organic matter (SOM) in soils and sediments. Fe-bearing clay minerals are widely distributed in these environments and often co-exist with lignin. While previous studies have reported the electron shuttling and donating roles of certain redox-active SOM in the dissimilatory reduction of structural Fe(III) in Fe-bearing clay minerals, the role of lignin in this process remains unknown. Here we studied this role by incubating an Fe-rich smectite (nontronite NAu-2) with two types of lignin (soluble and insoluble) in the absence and presence of an Fe(III)-reducing bacterium Shewanella putrefaciens CN32 under anaerobic condition. Labile carbon source (i.e., lactate) was added in some experiments as an extra electron donor. The results demonstrated that both soluble and insoluble lignins abiotically reduced structural Fe(III) in NAu-2. The reduction extent was proportional to lignin concentration. After abiotic reaction, lignin served as either electron shuttle or electron donor in the presence of CN32: (1) When lactate was present, lignin served as an electron shuttle to enhance the rate of Fe(III) reduction; (2) When lactate was absent, lignin served as an electron donor for Fe(III) reduction. Although the biotic Fe(III) reduction extents were similar in the presence of either soluble or insoluble lignin, the reduction rates with soluble lignin were always higher than those with insoluble lignin, likely owing to their different electron transfer mechanisms. After interaction with NAu-2 and/or CN32, soluble lignin structure largely remained intact, but with some decreases of humic/fulvic acid-like and protein-like compounds, aromatic functional groups (e.g., C-H, C=O, COOH), and aliphatic/aromatic compounds. An increase of semiquinone-like organic radicals was observed after lignin interaction with NAu-2. These chemical changes of lignin were likely coupled with reduction of structural Fe(III) in nontronite. The nontronite structure remained largely unchanged without much dissolution and mineral transformation. The findings of this study provide insights into the role of lignin in promoting mineral-microbe interactions and have significant implications for coupled Fe and C biogeochemical cycles in soils and sediments.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER); National Science Foundation (NSF)

Grant/Contract Number:: AC05-76RL01830; EAR-1148039; 51570; EAR 1148039

OSTI ID:: 1812535

Alternate ID(s):: OSTI ID: 1815051

Report Number(s):: PNNL-SA-156873

Journal Information:: Geochimica et Cosmochimica Acta, Vol. 307; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
59 BASIC BIOLOGICAL SCIENCES
58 GEOSCIENCES
Dissimilatory Fe(III) reduction
Electron donor
Electron shuttle
Lignin
Nontronite
Shewanella putrefaciens

Title: Lignin-enhanced reduction of structural Fe(III) in nontronite: Dual roles of lignin as electron shuttle and donor

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