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1.
J Hazard Mater ; 468: 133761, 2024 Apr 15.
Article En | MEDLINE | ID: mdl-38364580

Co-contaminants and complex subsurface conditions pose great challenges to site remediation. This study demonstrates the potential of electrokinetic bioremediation (EK-BIO) in treating co-contaminants of chlorinated solvents and heavy metals in low-permeability soils with elevated sulfate. EK-BIO columns were filled with field soils, and were fed by the electrolyte containing 20 mg/L trichloroethylene (TCE), 250 µM Cr(VI), 25 µM As(III), 10 mM lactate, and 10 mM sulfate. A dechlorinating consortium containing Dehalococcoides (Dhc) was injected several times during a 199-d treatment at ∼1 V/cm. Sulfate reduction, Cr/As immobilization, and complete TCE biodechlorination were observed sequentially. EK-BIO facilitated the delivery of lactate, Cr(VI)/As(III), and sulfate to the soils, creating favorable reductive conditions for contaminant removal. Supplementary batch experiments and metagenomic/transcriptomic analysis suggested that sulfate promoted the reductive immobilization of Cr(VI) by generating sulfide species, which subsequently enhanced TCE biodechlorination by alleviating Cr(VI) toxicity. The dechlorinating community displayed a high As(III) tolerance. Metagenomic binning analysis revealed the dechlorinating activity of Dhc and the potential synergistic effects from other bacteria in mitigating heavy metal toxicity. This study justified the feasibility of EK-BIO for co-contaminant treatment and provided mechanistic insights into EK-BIO treatment.


Chromium , Trichloroethylene , Biodegradation, Environmental , Sulfates , Soil , Sulfur Oxides , Lactic Acid
2.
Sci Total Environ ; 919: 170855, 2024 Apr 01.
Article En | MEDLINE | ID: mdl-38340822

Sediment oxidation by oxygen is ubiquitous, whereas the mechanisms of concurrent contaminant oxidation, particularly the temporal variation of chemical and biological oxidation, remain inadequately understood. This study investigated the oxidation of two contaminants (phenol and trichloroethylene) with different responses during the oxygenation of four natural sediments with different redox properties. Results showed that contaminant oxidation was initially dominated by hydroxyl radicals (•OH) (first stage), stabilized for different time for different sediments (second stage), and was re-started by microbial mechanism (third stage). In the first short stage, the contribution of chemical oxidation by •OH was mainly determined by the variation of sediment electron-donating capacity (EDC). In the second long stage, the stabilization time was dependent on sediment redox properties, that is, the abundance and growth of aerobic microbes capable of degrading the target contaminants. A more reduced sediment resulted in a higher extent of oxidation by •OH and a longer stabilization time. When the third stage of aerobic microbial oxidation was started, the contaminants like phenol that can be utilized by microbes can be oxidized quickly and completely, and those refractory contaminants like trichloroethylene remained unchanged. The study differentiates chemical and biological mechanisms for contaminant oxidation during sediment oxygenation.


Hydroxyl Radical , Trichloroethylene , Hydroxyl Radical/chemistry , Oxidation-Reduction , Phenol , Phenols
3.
Environ Sci Technol ; 57(12): 5046-5055, 2023 03 28.
Article En | MEDLINE | ID: mdl-36926893

Electrokinetic-enhanced bioremediation (EK-Bio), particularly bioaugmentation with injection of biodehalogenation functional microbes such as Dehalococcoides, has been documented to be effective in treating a low-permeability subsurface matrix contaminated with chlorinated ethenes. However, the spatio-temporal variations of indigenous microbial community and biodehalogenation activity of the background matrix, a fundamental aspect for understanding EK-Bio, remain unclear. To fill this gap, we investigated the variation of trichloroethylene (TCE) biodehalogenation activity in response to indigenous microbial community succession in EK-Bio by both column and batch experiments. For a 195 day EK-Bio column (∼1 V/cm, electrolyte circulation, lactate addition), biodehalogenation activity occurred first near the cathode (<60 days) and then spread to the anode (>90 days), which was controlled by electron acceptor (i.e., Fe(III)) competition and microbe succession. Amplicon sequencing and metagenome analysis revealed that iron-reducing bacteria (Geobacter, Anaeromyxobacter, Geothrix) were enriched within initial 60 d and were gradually replaced by organohalide-respiring bacteria (versatile Geobacter and obligate Dehalobacter) afterward. Iron-reducing bacteria required an initial long time to consume the competitive electron acceptors so that an appropriate reductive condition could be developed for the enrichment of organohalide-respiring bacteria and the enhancement of TCE biodehalogenation activity.


Microbiota , Trichloroethylene , Biodegradation, Environmental , Ferric Compounds , Bacteria , Soil , Permeability , Iron
4.
Environ Sci Pollut Res Int ; 30(11): 31188-31201, 2023 Mar.
Article En | MEDLINE | ID: mdl-36445524

Chlorinated solvents are widespread subsurface contaminants that are often present as complex mixtures. Complete biodegradation of mixed chlorinated solvents remains challenging because the optimal redox conditions for biodegradation of different chlorinated solvents differ significantly. In this study, anaerobic and aerobic conditions were integrated by electrolysis coupled with groundwater circulation for biodegradation of a mixture of chloroform (CF, 8.25 mg/L), 1,2-dichloroethane (DCA, 7.01 mg/L), and trichloroethylene (TCE, 4.56 mg/L). A two-dimensional tank was filled with field sandy and silty-clayed sediments to simulate aquifer conditions, a pair of electrodes was installed between an injection well and abstraction well, and groundwater circulation transported cathodic H2 and anodic O2 to produce multiple redox conditions. Microbial community analysis demonstrated that the system constructed a habitat suitable for the co-existence of aerobic and anaerobic microbes. After 50 days of treatment, 93.1%, 100%, and 87.3% of CF, 1,2-DCA, and TCE were removed without observed intermediates, respectively. Combined with compound specific isotope analysis, the degradation of 1,2-DCA and CF was mainly attributed to aerobic oxidation and reductive dechlorination, respectively, and TCE was removed by both aerobic and anaerobic biodegradation. Our findings provide a new and efficient strategy for in situ bioremediation of groundwater contaminated by mixed chlorinated solvents.


Groundwater , Trichloroethylene , Water Pollutants, Chemical , Biodegradation, Environmental , Water Pollutants, Chemical/analysis , Anaerobiosis , Trichloroethylene/analysis , Solvents , Electrolysis
5.
Article En | MEDLINE | ID: mdl-36078709

Increased concentrations of heavy metals in soil due to anthropogenic activities pose a considerable threat to human health and require constant attention. This study investigates the spatial distribution of heavy metals (Cd, Pb, Zn, Sb) and metalloids (As) in a typical alluvial-lacustrine transition basin and calculates the bioavailable forms of elements posing a direct threat. Qualitative and quantitative methods were used to identify the sources of contaminants, after which an ecological risk assessment was conducted. Total (T) As, Pb, and Zn decreased with the depth, whereas Cd and Sb increased in surface (0-20 cm) soil. Bioavailable (Bio) Cd and Pb in the topsoil were regulated by pH and organic matter, whereas Bio-Zn was regulated by soil pH. Within deeper soil layers, the combined effects of pH, organic matter, and clay contents regulated the bio-elements. The results of multiple methods and local investigation showed that TSb (65.3%) was mainly derived from mining activities, TCd (53.2%) and TZn (53.7%) were derived from direct pollution by industrial production and agricultural fertilizers, respectively, and TA (55.6%) was mainly derived from the soil parent material. TPb was related to vehicle exhaust emissions and atmospheric deposition from industrial activities. Although the potential ecological risk in the study area remains relatively low, there is a need for continuous monitoring of the potential ecological risks of Cd and Sb. This study can act as a reference for the prevention and mitigation of heavy metal contamination of alluvial-lacustrine transition basins.


Metals, Heavy , Soil Pollutants , Cadmium , China , Environmental Monitoring/methods , Farms , Humans , Lead , Metals, Heavy/analysis , Risk Assessment , Soil/chemistry , Soil Pollutants/analysis
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