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Record W2913727043 · doi:10.1021/acs.est.8b03717

Reductive Dehalogenation of Trichloromethane by Two Different <i>Dehalobacter restrictus</i> Strains Reveal Opposing Dual Element Isotope Effects

2019· article· en· W2913727043 on OpenAlexafffund
Benjamin Heckel, Elizabeth Phillips, Elizabeth A. Edwards, Barbara Sherwood Lollar, Martin Elsner, Michael Manefield, Matthew Lee

Bibliographic record

VenueEnvironmental Science & Technology · 2019
Typearticle
Languageen
FieldEnvironmental Science
TopicMicrobial bioremediation and biosurfactants
Canadian institutionsUniversity of Toronto
FundersNatural Sciences and Engineering Research Council of CanadaDeutsche ForschungsgemeinschaftHelmholtz-Gemeinschaft
KeywordsKinetic isotope effectChemistryIsotope analysisStereochemistryStable isotope ratioIsotopes of carbonIsotopeBiochemistryOrganic chemistryBiologyDeuteriumTotal organic carbon

Abstract

fetched live from OpenAlex

Trichloromethane (TCM) is a frequently detected and persistent groundwater contaminant. Recent studies have reported that two closely related Dehalobacter strains (UNSWDHB and CF) transform TCM to dichloromethane, with inconsistent carbon isotope effects (ε 13 C UNSWDHB = −4.3 ± 0.45‰; ε 13 C CF = −27.5 ± 0.9‰). This study uses dual element compound specific isotope analysis (C; Cl) to explore the underlying differences. TCM transformation experiments using strain CF revealed pronounced normal carbon and chlorine isotope effects (ε 13 C CF = −27.9 ± 1.7‰; ε 37 Cl CF = −4.2 ± 0.2‰). In contrast, small carbon and unprecedented inverse chlorine isotope effects were observed for strain UNSWDHB (ε 13 C UNSWDHB = −3.1 ± 0.5‰; ε 37 Cl UNSWDHB = 2.5 ± 0.3‰) leading to opposing dual element isotope slopes (λ CF = 6.64 ± 0.14 vs λ UNSWDHB = −1.20 ± 0.18). Isotope effects of strain CF were identical to experiments with TCM and Vitamin B 12 (ε 13 C Vitamin B12 = −26.0 ± 0.9‰, ε 37 Cl Vitamin B12 = −4.0 ± 0.2‰, λ Vitamin B12 = 6.46 ± 0.20). Comparison to previously reported isotope effects suggests outer-sphere-single-electron transfer or S N 2 as possible underlying mechanisms. Cell suspension and cell free extract experiments with strain UNSWDHB were both unable to unmask the intrinsic KIE of the reductive dehalogenase (TmrA) suggesting that enzyme binding and/or mass-transfer into the periplasm were rate-limiting. Nondirected intermolecular interactions of TCM with cellular material were ruled out as reason for the inverse isotope effect by gas/water and gas/hexadecane partitioning experiments indicating specific, yet uncharacterized interactions must be operating prior to catalysis.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame machine prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: metacan-v3-hybrid-931329e0061cValidation status: machine_predicted_unvalidated
Candidate categoriesnone
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.005
Threshold uncertainty score0.010

Distilled classifier scores by category (both heads)

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0000.000
Meta-epidemiology (broad)0.0000.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0000.000
Research integrity0.0000.000
Insufficient payload (model declined to judge)0.0000.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.004
GPT teacher head0.207
Teacher spread0.204 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.

The models applied no category: nothing in the taxonomy fit this work.
Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations46
Published2019
Admission routes2
Has abstractyes

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