Role of clay-associated humic substances in catalyzing bioreduction of structural Fe(III) in nontronite by Shewanella putrefaciens CN32

Zuo, Hongyan; Kukkadapu, Ravi; Zhu, Zihua; Ni, Shuisong; Huang, Liuqin; Zeng, Qiang; Liu, Chongxuan; Dong, Hailiang

doi:10.1016/j.scitotenv.2020.140213

Title: Role of clay-associated humic substances in catalyzing bioreduction of structural Fe(III) in nontronite by Shewanella putrefaciens CN32

Journal Article · Fri Jun 19 00:00:00 EDT 2020 · Science of the Total Environment

DOI:https://doi.org/10.1016/j.scitotenv.2020.140213· OSTI ID:1646332

Zuo, Hongyan ^[1]; Kukkadapu, Ravi ^[2]; Zhu, Zihua ^[2]; Ni, Shuisong ^[3]; Huang, Liuqin ^[4]; Zeng, Qiang ^[5]; Liu, Chongxuan ^[6]; Dong, Hailiang ^[1]

Miami Univ., Oxford, OH (United States). Dept. of Geology and Environmental Earth Science
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, Wuhan (China). State Key Laboratory of Biogeology and Environmental Geology
China Univ. of Geosciences, Beijing (China). State Key Laboratory of Biogeology and Environmental Geology
Southern Univ. of Science and Technology, Shenzen (China). School of Environmental Science and Engineering

Previous studies have shown that humic substances can serve as electron shuttle to catalyze bioreduction of structural Fe(III) in clay minerals, but it is unclear if clay-sorbed humic substances can serve the same function. It is unknown if the electron shuttling function is dependent on electron donor type and if humic substances undergo change as a result. Here, humic acid (HA) and fulvic acid (FA) were sorbed onto nontronite (NAu-2) surface. Structural Fe(III) in HA- and FA-coated NAu-2 samples was bioreduced by Shewanella putrefaciens CN32 using H₂ and lactate as electron donors. The results showed a contrasting effect of humic substances on bioreduction of structural Fe(III), depending on the electron donor type. With H₂ as electron donor, humic substances had little effect on bioreduction of Fe(III) (the reduction extent: 26.2%, 27.4%, 29.3% for HA-coated, FA-coated, and uncoated NAu-2, respectively). In contrast, these substances significantly enhanced bioreduction of Fe(III) with lactate as electron donor (the reduction extent: 20.2%, 20.7%, 11.5% for HA-coated, FA-coated, and uncoated NAu-2, respectively). This contrasting behavior is likely caused by the difference in reaction free energy and electron transport process between H₂ and lactate. When H₂ served as electron donor, more energy was released than when lactate served as electron donor. In addition, because of different cellular locations of lactate dehydrogenase (inner membrane) and H₂ hydrogenase (the periplasm), electrons generated by H₂ hydrogenase may pass through the electron transport chain more rapidly than those generated from lactate dehydrogenase. Through their functions as electron shuttle and/or carbon source, clay-sorbed HA/FA underwent partial transformation to amino acids and other compounds. The availability of external carbon source played an important role in the amount and type of secondary product generation. These results have important implications for coupled iron and carbon biogeochemical cycles in clay- and humic substance-rich environments.

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Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States). Environmental Molecular Sciences Laboratory (EMSL)

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

Grant/Contract Number:: AC05-76RL01830; EAR-1656988; EAR-0722807

OSTI ID:: 1646332

Alternate ID(s):: OSTI ID: 1682472

Report Number(s):: PNNL-SA-153739

Journal Information:: Science of the Total Environment, Vol. 741; ISSN 0048-9697

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Comparing electron donating/accepting capacities (EDC/EAC) between crop residue-derived dissolved black carbon and standard humic substances Zheng, Xiaojian; Liu, Yafang; Fu, Heyun Science of The Total Environment, Vol. 673 https://doi.org/10.1016/j.scitotenv.2019.04.022	journal	July 2019

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