Microbially Driven Fenton Reaction for Degradation of the Widespread Environmental Contaminant 1,4-Dioxane

Sekar, Ramanan; DiChristina, Thomas J.

doi:10.1021/es503454a

Cited by 82 publications

(60 citation statements)

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“…Since xylose is a lignocellulose degradation product, this study expands the potential substrates to include lignocellulosic biomass. Metabolism of multiple carbon sources, such as glucose, glycerol, and xylose, by S. oneidensis has the potential to improve the efficiency of electricity generation, biofuel production, and bioremediation of toxic contaminants (16,17,50). …”

Section: Discussionmentioning

confidence: 99%

Activation of an Otherwise Silent Xylose Metabolic Pathway in Shewanella oneidensis

Sekar

Shin

DiChristina

2016

Appl Environ Microbiol

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Shewanella oneidensis is unable to metabolize the sugar xylose as a carbon and energy source. In the present study, an otherwise silent xylose catabolic pathway was activated in S. oneidensis by following an adaptive evolution strategy. Genome-wide scans indicated that the S. oneidensis genome encoded two proteins similar to the xylose oxido-reductase pathway enzymes xylose reductase (SO_0900) and xylulokinase (SO_4230), and purified SO_0900 and SO_4230 displayed xylose reductase and xylulokinase activities, respectively. The S. oneidensis genome was missing, however, an Escherichia coli XylE-like xylose transporter. After 12 monthly transfers in minimal growth medium containing successively higher xylose concentrations, an S. oneidensis mutant (termed strain XM1) was isolated for the acquired ability to grow aerobically on xylose as a carbon and energy source. Wholegenome sequencing indicated that strain XM1 contained a mutation in an unknown membrane protein (SO_1396) resulting in a glutamine-to-histidine conversion at amino acid position 207. Homology modeling demonstrated that the Q207H mutation in SO_1396 was located at the homologous xylose docking site in XylE. The expansion of the S. oneidensis metabolic repertoire to xylose expands the electron donors whose oxidation may be coupled to the myriad of terminal electron-accepting processes catalyzed by S. oneidensis. Since xylose is a lignocellulose degradation product, this study expands the potential substrates to include lignocellulosic biomass. IMPORTANCEThe activation of an otherwise silent xylose metabolic system in Shewanella oneidensis is a powerful example of how accidental mutations allow microorganisms to adaptively evolve. The expansion of the S. oneidensis metabolic repertoire to xylose expands the electron donors whose oxidation may be coupled to the myriad of terminal electron-accepting processes catalyzed by S. oneidensis. Since xylose is a lignocellulose degradation product, this study expands the potential substrates to include lignocellulosic biomass. Xylose is one of the primary products of lignocellulose degradation and, after glucose, is the second most abundant carbohydrate in nature. The xylose polymer xylan is the primary constituent of hemicellulose, which comprises approximately 17% of the dry weight of hardwoods and up to 31% of plants (1). Xylose catabolism is a key component of sustainable processes that produce useful secondary products from lignocellulosic biomass (2-4). Xylose catabolism is also of commercial interest because xylose conversion to useful secondary chemicals such as bioethanol and biodegradable plastics can reduce losses associated with lignocellulose bioprocessing (5, 6). Industrially important by-products of xylose metabolism include xylitol, which is used as a natural sweetener in the food and confectionary industries (7).Xylose metabolic pathways include the oxido-reductase, isomerase, and Weimberg-Dahms pathways (Fig. 1) (1, 8). Extracellular xylose is transported inside the cell via the ATP-bindi...

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Section: Discussionmentioning

confidence: 99%

Activation of an Otherwise Silent Xylose Metabolic Pathway in Shewanella oneidensis

Sekar

Shin

DiChristina

2016

Appl Environ Microbiol

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“…Conventional Fenton reaction-generated HO˙radicals oxidatively degrade a number of hazardous compounds, including chlorinated aliphatic and aromatic compounds (34), pentachlorophenol (PCP) (35,36), PCE (24), TCE (1,5,23,26,33), 1,1,2-trichloroethane (TCA) (37), 1,4-dioxane (32), and petroleum hydrocarbons (38). Conventional Fenton reaction-driven transformation of TCE, PCE, and 1,4-dioxane is limited, however, by the high concentrations of the Fenton reagents Fe(II) and H 2 O 2 that must be continuously supplied to produce HO˙radicals and drive TCE, PCE, and 1,4-dioxane transformation (1,24).…”

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“…UV irradiation is often employed to induce Fe(III) rereduction and photolytic radical production in photo-Fenton systems. The UV irradiation systems, however, are limited by UV light penetration, and H 2 O 2 must still be continuously supplied to drive the conventional Fenton reaction (32). Microbially driven Fenton reactions that alternately produce the Fenton reagents H 2 O 2 (via microbial O 2 respiration) and Fe(II) [via microbial Fe(III) reduction] alleviate the need for continual addition of H 2 O 2 and Fe(II) to drive HO˙radical production (12,17,32,40).…”

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confidence: 99%

“…The UV irradiation systems, however, are limited by UV light penetration, and H 2 O 2 must still be continuously supplied to drive the conventional Fenton reaction (32). Microbially driven Fenton reactions that alternately produce the Fenton reagents H 2 O 2 (via microbial O 2 respiration) and Fe(II) [via microbial Fe(III) reduction] alleviate the need for continual addition of H 2 O 2 and Fe(II) to drive HO˙radical production (12,17,32,40). The Fe(III)-reducing facultative anaerobe Shewanella oneidensis was recently employed to drive the Fenton reaction for oxidative degradation of PCP and 1,4-dioxane (32,36).…”

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confidence: 99%

“…Microbially driven Fenton reactions that alternately produce the Fenton reagents H 2 O 2 (via microbial O 2 respiration) and Fe(II) [via microbial Fe(III) reduction] alleviate the need for continual addition of H 2 O 2 and Fe(II) to drive HO˙radical production (12,17,32,40). The Fe(III)-reducing facultative anaerobe Shewanella oneidensis was recently employed to drive the Fenton reaction for oxidative degradation of PCP and 1,4-dioxane (32,36). In the S. oneidensis-driven Fenton reaction, batch liquid cultures were amended with Fe(III) and 1,4-dioxane and subsequently exposed to alternating anaerobic and aerobic conditions.…”

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Simultaneous Transformation of Commingled Trichloroethylene, Tetrachloroethylene, and 1,4-Dioxane by a Microbially Driven Fenton Reaction in Batch Liquid Cultures

Sekar

Taillefert

DiChristina

2016

Appl Environ Microbiol

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Improper disposal of 1,4-dioxane and the chlorinated organic solvents trichloroethylene (TCE) and tetrachloroethylene (also known as perchloroethylene [PCE]) has resulted in widespread contamination of soil and groundwater. In the present study, a previously designed microbially driven Fenton reaction system was reconfigured to generate hydroxyl (HO˙) radicals for simultaneous transformation of source zone levels of single, binary, and ternary mixtures of TCE, PCE, and 1,4-dioxane. The reconfigured Fenton reaction system was driven by fed batch cultures of the Fe(III)-reducing facultative anaerobe Shewanella oneidensis amended with lactate, Fe(III), and contaminants and exposed to alternating anaerobic and aerobic conditions. To avoid contaminant loss due to volatility, the Fe(II)-generating, hydrogen peroxide-generating, and contaminant transformation phases of the microbially driven Fenton reaction system were separated. The reconfigured Fenton reaction system transformed TCE, PCE, and 1,4-dioxane either as single contaminants or as binary and ternary mixtures. In the presence of equimolar concentrations of PCE and TCE, the ratio of the experimentally derived rates of PCE and TCE transformation was nearly identical to the ratio of the corresponding HO˙radical reaction rate constants. The reconfigured Fenton reaction system may be applied as an ex situ platform for simultaneous degradation of commingled TCE, PCE, and 1,4-dioxane and provides valuable information for future development of in situ remediation technologies. IMPORTANCE A microbially driven Fenton reaction system [driven by the Fe(III)-reducing facultative anaerobe S. oneidensis] was reconfigured to transform source zone levels of TCE, PCE, and 1,4-dioxane as single contaminants or as binary and ternary mixtures.The microbially driven Fenton reaction may thus be applied as an ex situ platform for simultaneous degradation of at least three (and potentially more) commingled contaminants. Additional targets for ex situ and in situ degradation by the microbially driven Fenton reaction developed in the present study include multiple combinations of environmental contaminants susceptible to attack by Fenton reaction-generated HO˙radicals, including commingled plumes of 1,4-dioxane, pentachlorophenol (PCP), PCE, TCE, 1,1,2-trichloroethane (TCA), and perfluoroalkylated substances (PFAS).T he chlorinated organic solvents trichloroethylene (TCE) and tetrachloroethylene (also known as perchloroethylene [PCE]) have been historically employed as solvents in a variety of industrial processes, including vapor degreasing of metal surfaces, paint stripping, and dry cleaning (1, 2). TCE and PCE are carcinogenic, and improper disposal practices at industrial sites have resulted in widespread contamination of soil and groundwater (1-6). Due to their high density and low aqueous phase solubility, TCE and PCE are also highly persistent in contaminated environments (3, 4). The potential carcinogen 1,4-dioxane is generally employed as a stabilizer for TCE and PCE i...

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Application ofShewanellato Water Treatment Issues

Szeinbaum¹,

Toporek²,

Shin³

et al. 2019

Encyclopedia of Water

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Shewanella drives a variety of environmentally important processes, including the biogeochemical cycling of carbon, metals, metalloids, and radionuclides. The ability of Shewanella to deliver electrons extracellularly also renders this genus valuable for applications of contaminant remediation and energy generation in water treatment processes. Although the first Shewanella species was isolated and studied as a model metal‐reducing microorganism over thirty years ago, only recently has research focused on employing Shewanella to drive water treatment processes. This article examines current and prospective applications of Shewanella to water treatment issues, highlighting biochemical details associated with each technology. The technologies include the remediation of metal‐contaminated environments, the generation of electricity from wastewater streams, the removal of hazardous contaminants under anaerobic conditions, and precious metal recovery in combination with formation of novel biocatalysts.

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Microbially Driven Fenton Reaction for Degradation of the Widespread Environmental Contaminant 1,4-Dioxane

Cited by 82 publications

References 56 publications

Activation of an Otherwise Silent Xylose Metabolic Pathway in Shewanella oneidensis

Activation of an Otherwise Silent Xylose Metabolic Pathway in Shewanella oneidensis

Simultaneous Transformation of Commingled Trichloroethylene, Tetrachloroethylene, and 1,4-Dioxane by a Microbially Driven Fenton Reaction in Batch Liquid Cultures

Application ofShewanellato Water Treatment Issues

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