Vanadium Chloroperoxidases: The Missing Link in the Formation of Chlorinated Compounds and Chloroform in the Terrestrial Environment?

Wever, Ron; Barnett, Phil

doi:10.1002/asia.201700420

Cited by 37 publications

(23 citation statements)

References 114 publications

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“…In addition, simultaneous and rapid dechlorination of Cl org in soils was also confirmed (Montelius et al 2016 ). Enzymatic control of chlorination processes has been described (van Pee and Unversucht 2003 ; Bastviken et al 2009 ; Wever and Barnett 2017 ), and the genetic capacity to carry out chlorination is widespread among prokaryotes and eukaryotes alike (Bengtson et al 2009 ; Bengtson et al 2013 ; Weigold et al 2016 ). The extensive natural chlorination processes in soil suggest that the Cl turnover likely is linked to common ecosystem processes.…”

Section: Introductionmentioning

confidence: 99%

Chlorine cycling and the fate of Cl in terrestrial environments

Svensson

Kylin

Montelius

et al. 2021

Environ Sci Pollut Res

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Chlorine (Cl) in the terrestrial environment is of interest from multiple perspectives, including the use of chloride as a tracer for water flow and contaminant transport, organochlorine pollutants, Cl cycling, radioactive waste (radioecology; 36Cl is of large concern) and plant science (Cl as essential element for living plants). During the past decades, there has been a rapid development towards improved understanding of the terrestrial Cl cycle. There is a ubiquitous and extensive natural chlorination of organic matter in terrestrial ecosystems where naturally formed chlorinated organic compounds (Clorg) in soil frequently exceed the abundance of chloride. Chloride dominates import and export from terrestrial ecosystems while soil Clorg and biomass Cl can dominate the standing stock Cl. This has important implications for Cl transport, as chloride will enter the Cl pools resulting in prolonged residence times. Clearly, these pools must be considered separately in future monitoring programs addressing Cl cycling. Moreover, there are indications that (1) large amounts of Cl can accumulate in biomass, in some cases representing the main Cl pool; (2) emissions of volatile organic chlorines could be a significant export pathway of Cl and (3) that there is a production of Clorg in tissues of, e.g. plants and animals and that Cl can accumulate as, e.g. chlorinated fatty acids in organisms. Yet, data focusing on ecosystem perspectives and combined spatiotemporal variability regarding various Cl pools are still scarce, and the processes and ecological roles of the extensive biological Cl cycling are still poorly understood.

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Section: Introductionmentioning

confidence: 99%

Chlorine cycling and the fate of Cl in terrestrial environments

Svensson

Kylin

Montelius

et al. 2021

Environ Sci Pollut Res

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“…In the water column, DCM concentrations peak along with chlorophyll concentrations (Ooki & Yokouchi, 2011), consistent with production by phytoplankton and the abiotic chlorination of planktonic iodo- and bromomethanes (Ooki & Yokouchi, 2011). DCM is detected beneath the photic zone (Ooki & Yokouchi, 2011), suggesting that mixing events carry DCM into deeper waters, or other sources of DCM exist in the deep ocean, possibly hydrothermal vents (Eklund et al, 1988; Isidorov et al, 1990; Jordan et al, 2000) or settling dead biomass (Wever & Barnett, 2017). Importantly, analysis of ETNP OMZ samples using targeted qPCR assays led to much high detection rate (9 of 11) than was obtained by metagenome analyses (16 of 90).…”

Section: Discussionmentioning

confidence: 99%

Global distribution of anaerobic dichloromethane degradation potential

Murdoch

Chen

Murdoch

et al. 2021

Preprint

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Anthropogenic activities and natural processes release dichloromethane (DCM), a toxic chemical with substantial ozone-depleting capacity. Specialized anaerobic bacteria metabolize DCM; however, the genetic basis for this process has remained elusive. Comparative genomics of the three known anaerobic DCM-degrading bacterial species revealed a homologous gene cluster, designated the methylene chloride catabolism (mec) gene cassette, comprising eight to ten genes with predicted 79.6 – 99.7% amino acid identity. Functional annotation identified genes encoding a corrinoid-dependent methyltransferase system, and shotgun proteomics applied to two DCM-catabolizing cultures revealed high expression of proteins encoded on the mec gene cluster during anaerobic growth with DCM. In a DCM-contaminated groundwater plume, the abundance of mec genes strongly correlated with DCM concentrations (R2 = 0.71 – 0.85) indicating their value as process-specific bioremediation biomarkers. mec gene clusters were identified in metagenomes representing peat bogs, the deep subsurface, and marine ecosystems including oxygen minimum zones (OMZs), suggesting DCM turnover in diverse habitats. The broad distribution of anaerobic DCM catabolic potential suggests a relevant control function for emissions to the atmosphere, and a role for DCM as a microbial energy source in critical zone environments. The findings imply that the global DCM flux might be far greater than emission measurements suggest.ImportanceDichloromethane (DCM) is an increasing threat to stratospheric ozone with both anthropogenic and natural emission sources. Anaerobic bacterial metabolism of DCM has not yet been taken into consideration as a factor in the global DCM cycle. The discovery of the mec gene cassette associated with anaerobic bacterial DCM metabolism and its widespread distribution in environmental systems highlight a strong attenuation potential for DCM. Knowledge of the mec cassette offers new opportunities to delineate DCM sources, enables more robust estimates of DCM fluxes, supports refined DCM emission modeling and simulation of the stratospheric ozone layer, reveals a novel, ubiquitous C1 carbon metabolic system, and provides prognostic and diagnostic tools supporting bioremediation of groundwater aquifers impacted by DCM.

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“…Enzyme activity assay . To assess Ci VCPO activity, a standardised assay reported previously was used . In short: in a disposable UV plastic cuvette a solution (1 mL) containing 50 μM monochlorodimedone (MCD), 1 mM H 2 O 2 , 0.5 mM NaBr, 100 μM Na 3 VO 4 in 50 mM sodium citrate (pH 5.6) was prepared.…”

Section: Methodsmentioning

confidence: 99%

Towards Preparative Chemoenzymatic Oxidative Decarboxylation of Glutamic Acid

But

Wever

et al. 2020

ChemCatChem

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The chemoenzymatic oxidative decarboxylation of glutamic acid to the corresponding nitrile using the vanadium chloroperoxidase from Curvularia inaequalis (CiVCPO) as HOBr generation catalysts has been investigated. Product inhibition was identified as major limitation. Nevertheless, 1630000 turnovers and kcat of 75 s−1 were achieved using 100 mM glutamate. The semi‐preparative enzymatic oxidative decarboxylation of glutamate was also demonstrated.

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Vanadium Chloroperoxidases: The Missing Link in the Formation of Chlorinated Compounds and Chloroform in the Terrestrial Environment?

Cited by 37 publications

References 114 publications

Chlorine cycling and the fate of Cl in terrestrial environments

Chlorine cycling and the fate of Cl in terrestrial environments

Global distribution of anaerobic dichloromethane degradation potential

Towards Preparative Chemoenzymatic Oxidative Decarboxylation of Glutamic Acid

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