Effect of groundwater biogeochemistry on zero valent iron nanoparticles: Role of sulfidation and bacteria on reductive dechlorination
Bibliographic record
Abstract
Accidental spills and past improper disposal practices of chlorinated solvents have led to widespread soil and groundwater contamination. Drinking water standards for trichloroethylene (TCE) and many other chlorinated organic contaminants are in the range of 5 µg/L and these compounds have received extensive regulatory attention because these compounds are often carcinogenic and neurotoxic. Direct injection of reactive nanoscale zerovalent iron particles (NZVI) is considered to be a promising approach for remediation of chlorinated compounds. NZVI is a strong reducing agent that can effectively transform TCE and other chlorinated organic compounds to non-toxic end products. The objective of the research was to assess various biogeochemical conditions on the reactivity of iron nanoparticles in particular sulfidation of NZVI for remediation of TCE. In addition, the feasibility of coupled NZVI-based remediation and bioremediation using polymer-coated bimetallic NZVI and a dechlorinating mixed culture consortia (KB-1) was investigated. We demonstrated that the extent of sulfidation of NZVI enhances the rate of dechlorination of TCE compared to non-sulfidated NZVI, and this enhancement depends on the Fe/S molar ratio of the sulfidated NZVI particles. Batch experiments where TCE was reacted with NZVI sulfidated to different extents (Fe/S molar ratios 0.62 to 66) showed that the surface-area normalized first-order TCE degradation rate constant increased 40 fold compared to non-sulfidated NZVI. FX-ray photoelectron spectroscopy analyses showed formation of a surface layer of FeS and FeS2. This indicates sulfide ions reacted with NZVI iron sulfide on surface of S-NZVI. We propose that more electrons are preferentially conducted from sulfidated NZVI than from unamended NZVI to TCE, likely because of greater binding affinity of TCE on the reactive sites of the iron sulfide outer layer. Aging of sulfidated iron nanoparticles (S-NZVI) and their influence on rate of TCE dechlorination was compared to the aged non-sulfidated NZVI. Long-term experiments indicate that pseudo-first order H2 evolution rate constant for non-sulfidated NZVI was 0.092 ± 0.005 d-1 and was significantly higher than the S-NZVI (Fe/S=25) at 0.051 ± 0.005 h-1. This difference in hydrogen evolved corresponds to the amount of reactive Fe(0) consumed in the absence of TCE. To further support, the efficacy of long-term reactivity S-NZVI batch TCE degradation experiment with anaerobically aged S-NZVI (40 days) degraded significantly more TCE than the non-sulfidated NZVI. Bimetallic, palladium-doped iron nanoparticles (Pd-NZVI) are capable of rapid transformation of higher initial TCE concentration, and the ability to form rapid H2 (electron donor for bacteria) may facilitate TCE biodegradation. Dehalococcoides are the only species of bacteria that are capable of degrading TCE completely to ethene under anaerobic conditions. Therefore, we investigated the interaction of carboxymethyl cellulose (CMC) stabilized palladium (Pd-NZVI) on the dechlorinating mixed culture KB-1 for reductive dechlorination of 1, 2 dichloroethane (DCA). Results suggest that systems with CMC alone as a sole carbon source and electron donor were capable of degrading 1, 2-DCA, and methane formation. The microcosms with KB-1 and polymer coated Pd-NZVI degraded 1, 2-DCA at a significantly higher rate constant compared to KB-1 and CMC systems. In addition, methanogenesis by KB-1 showed no statistically significant difference in the methane formation rate constants between Pd-CMC-NZVI and CMC only systems.Overall, this research demonstrates NZVI reactivity towards TCE and its longevity (efficacy) under anaerobic conditions can be enhanced with sulfidation. In addition, this research also shows that CMC stabilized bimetallic NZVI, is not inhibitory to Dehalococcoides spp. and could promote complete bioremediation.
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.001 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
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.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
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".