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Mechanism of biochar functional groups in the catalytic reduction of tetrachloroethylene by sulfides Texto completo
2022
Yang, Yadong | Piao, Yunxian | Wang, Ruofan | Su, Yaoming | Qiu, Jinrong | Liu, Na
In recent years, biochar has become of considerable interest for environmental applications, it can be used as a catalyst for sulfides reduction of perchloroethylene, but the crucial role of biochar properties played in catalyzing dechlorination remained ambiguous investigation. To pinpoint the critical functional groups, the modified biochars were respectively produced by HNO₃, KOH and H₂O₂ with similar dimensional structures but different functional groups. Combined with the adsorption and catalytic results of different biochars, the acid-modified biochar had the best catalytic performance (99.9% removal) due to the outstanding specific surface area and ample functional groups. According to characterization and DFT results, carboxyl and pyridine nitrogen exhibited a positive correlation with the catalytic rate, indicating that their contribution to catalytic performance. Customizing biochar with specific functional groups removed depth demonstrated that the carboxyl was essential component. Further, alkaline condition was conducive to catalytic reduction, while tetrachloroethylene cannot be reduced under acidic conditions, because HS⁻ and S²⁻ mainly existed in alkaline environment and the sulfur-containing nucleophilic structure formed with biochar was more stable under this condition. Overall, this study opens new perspectives for in situ remediation by biochar in chlorinated olefin polluted anoxic environment and promotes our insight of modifying for biochar catalyst design.
Mostrar más [+] Menos [-]Bacterial communities as indicators of environmental pollution by POPs in marine sediments Texto completo
2021
Rodríguez, Juanjo | Gallampois, Christine M.J. | Haglund, Peter | Timonen, Sari | Rowe, Owen
Decades of intensive discharge from industrial activities into coastal systems has resulted in the accumulation of a variety of persistent organic pollutants (POPs) in marine waters and sediments, having detrimental impacts on aquatic ecosystems and the resident biota. POPs are among the most hazardous chemicals originating from industrial activities due to their biotoxicity and resistance to environmental degradation. Bacterial communities are known to break down many of these aromatic compounds, and different members of naturally occurring bacterial consortia have been described to work in syntrophic association to thrive in heavily contaminated waters and sediments, making them potential candidates as bioindicators of environmental pollution. In this study environmental, sampling was combined with chemical analysis of pollutants and high-resolution sequencing of bacterial communities using Next Generation Sequencing molecular biology tools. The aim of the present study was to describe the bacterial communities from marine sediments containing high loads of POPs and to identify relevant members of the resident microbial communities that may act as bioindicators of contamination. Marine sediments were collected from a coastal bay area of the Baltic Sea historically influenced by intense industrial activity, including metal smelting, oil processing, and pulp and paper production. Different types of POPs were detected at high concentrations. Fiberbank sediments, resulting from historic paper industry activity, were found to harbour a clearly distinct bacterial community including a number of bacterial taxa capable of cellulolytic and dechlorination activities. Our findings indicate that specific members of the bacterial communities thrive under increasing levels of POPs in marine sediments, and that the abundances of certain taxa correlate with specific POPs (or groups), which could potentially be employed in monitoring, status assessment and environmental management purposes.
Mostrar más [+] Menos [-]Innovative mycoremediation technique for treating unsterilized PCDD/F-contaminated field soil and the exploration of chlorinated metabolites Texto completo
2021
Kaewlaoyoong, Acharee | Chen, Jenq-Renn | Cheng, Chih-Yu | Lin, Chitsan | Cheruiyot, Nicholas Kiprotich | Sriprom, Pongsert
Mycoremediation of unsterilized PCDD/F-contaminated field soil was successfully demonstrated by solid-state fermentation coupled with Pleurotus pulmonarius utilizing a patented incubation approach. The experiments were carried out in four setups with two as controls. The contaminated soil was homogenously mixed with solid inocula, 1:0.5 dry w/w, resulting in an initial concentration of 4432 ± 623 ng WHO-TEQ kg⁻¹. After a 30-day incubation under controlled conditions, the overall removal (approx. 60%) was non-specific. The removal was attributed to degradation by extracellular ligninolytic enzymes and uptake into the fruiting tissue (~110 ng WHO-TEQ kg⁻¹ of mushroom). Furthermore, less recalcitrant chlorinated metabolites were found, implying ether bond cleavage and dechlorination happened during the mycoremediation. These metabolites resulted from the complex interaction between P. pulmonarius and the indigenous microbes from the unsterilized soil. This study provides a new step toward scaling up this mycoremediation technique to treat unsterilized PCDD/F-contaminated field soil.
Mostrar más [+] Menos [-]Crop-dependent root-microbe-soil interactions induce contrasting natural attenuation of organochlorine lindane in soils Texto completo
2020
Feng, Jiayin | Shentu, Jue | Zhu, Yanjie | Tang, Caixian | He, Yan | Xu, Jianming
Plant-specific root-microbe-soil interactions play an indisputable role in microbial adaptation to environmental stresses. However, the assembly of plant rhizosphere microbiomes and their feedbacks in modification of pollution alleviation under organochlorine stress condition is far less clear. This study examined the response of root-associated bacterial microbiomes to lindane pollution and compared the dissipation of lindane in maize-cultivated dry soils and rice-cultivated flooded soils. Results showed that lindane pollution dramatically altered the microbial structure in the rhizosphere soil of maize but had less influence on the microbial composition in flooded treatments regardless of rice growth, when the reductive dechlorination of lindane was actively coupled with natural redox processes under anaerobic conditions. After 30 days of plant growth, lindane residues dissipated much faster in anaerobic than in aerobic environments, with only 1.08 mg kg⁻¹ lindane remaining in flooded control compared to 12.79 mg kg⁻¹ in dry control soils. Compared to the corresponding unplanted control, maize growth significantly increased, but rice growth slightly decreased the dissipation of lindane. Our study suggests that opposite impacts would lead to the self-purification of polluted soils during the growth of xerophytic maize and hygrocolous rice. This was attributed to the contrasting belowground micro-ecological processes regarding protection of root tissues and thereby assembly of rhizosphere microbiomes shaped by the xerophytic and hygrocolous crops under different water managements, in response to lindane pollution.
Mostrar más [+] Menos [-]Deciphering microbiomes in anaerobic reactors with superior trichloroethylene dechlorination performance at low pH conditions Texto completo
2020
Chen, Wei-Yu | Wu, Jer-Horng | Chu, Shun-Chieh
Different pH conditions have been demonstrated to affect the activities of dechlorinating populations participating in the successive dechlorination of trichloroethylene to ethylene. However, the mechanism of the effect of pH conditions on the assembly of dechlorinating populations and their relations to the structure, function, and dynamics of the microbiome are unclear. In this study, we evaluated the effects of pH on microbiomes assembled in anaerobic trichloroethylene-dechlorinating reactors under neutral (pH 7.2), acidic (pH 6.2), and alkaline (pH 8.2) conditions. The results revealed that among the reactors, the acidic reactor had the highest efficiency for dechlorination without accumulation of dechlorinated metabolites, even at high loading rates. The results of high-throughput sequencing of the 16S rRNA gene indicated that the microbiomes in the 3 reactors underwent varied dynamic succession. The acidic reactor harbored a higher degree of complex microbes, dechlorinator diversity, and abundance of the Victoria subgroup of Dehalococcoides (1.2 ± 0.1 × 10⁶ cell/mL), which were approximately 10–10²-fold higher than those at neutral and alkaline conditions. The pH settings altered species–species connectivity and complexity of microbial interaction networks, with more commensal interactions in the dechlorinators of the acidic reactor. As predicted, abundances of several functional gene categories were in strong linearity with pH values, and the microbiome possessed significantly more abundant functions in the acidic reactor (P < 0.001), such as potentially stimulating hydrogen production, cobalamin synthesis, cobalt transport, transport and metabolism of amino acids and secondary metabolites, cell motility, and transcription. All results of microbiomic analyses consistently revealed the observed superior dechlorination process and suggested an association of the reductive dechlorination process with the pH-dependent microbiome. The results of this study provide a new insight into the trichloroethylene dechlorination with regards to pH, and they will be useful for improving bioremediation and management of trichloroethylene-contaminated sites.
Mostrar más [+] Menos [-]Acceleration of perchloroethylene dechlorination by extracellular secretions from Microbacterium in a mixed culture containing Desulfitobacterium Texto completo
2019
Wan, Jixing | Chen, Chen | Chen, Jingwen | Miao, Qianyu | Liu, Yindong | Ye, Junxiang | Chen, Kezhen | Jin, Yiying | Tang, Xianjin | Shen, Chaofeng
The study was conducted to demonstrate the influence of extracellular secretions from Microbacterium on the reductive dechlorination of tetrachloroethene (PCE). A series of mixed cultures were established from a paddy soil sample. In the mixed cultures amended with extracellular secretions from Microbacterium, PCE was rapidly and completely converted into cis-1,2-dichloroethene (cis-DCE) and trans-1,2-dichloroethene (trans-DCE) within 40 days. The unamended mixed cultures showed weak signs of dechlorination after a pronounced lag phase, and trichloroethene (TCE) was accumulated as a major end product. This result means that amendment with extracellular secretions from Microbacterium shortened the lag phase, increased the dechlorination velocity and promoted the production of less-chlorinated chloroethene. The results were corroborated by defined subculture experiments, which proved that microorganisms from unamended mixed cultures could also be stimulated by extracellular secretions from Microbacterium. Desulfitobacterium was identified as the main dechlorinating population in all mixed cultures by direct PCR. Additionally, the 16S rRNA gene copies of Desulfitobacterium increased by one or two orders of magnitude with PCE dechlorination, which provided corroborative evidence for the identification result. The volatile fatty acids were monitored, and most interestingly, a close association between propionate oxidation and dechlorination was found, which has rarely been mentioned before. It was assumed that the oxidation of propionate provided hydrogen for dechlorination, while dechlorination facilitated the shift of the reaction toward propionate oxidation by reducing the partial pressure of hydrogen.
Mostrar más [+] Menos [-]Redox properties and dechlorination capacities of landfill-derived humic-like acids Texto completo
2019
Xiao, Xiao | Xi, Bei-Dou | He, Xiao-Song | Zhang, Hui | Li, Yan-Hong | Pu, Shengyan | Liu, Si-Jia | Yu, Min-Da | Yang, Chao
Electron transfer capacities (ETC) of humic-like acids (HLA) and their effects on dechlorination are dependent on their redox-active properties. Aging and minerals can affect the chemical compositions and structures of HLA. However, the underlying mechanism and the impacts on the dechlorination capacities of HLA are poorly understood. We investigated how redox properties change in association with the intrinsic chemical natures and exterior minerals of the HLA extracted from landfilled solid wastes. Furthermore, the ETC of the landfill-derived HLA could be strengthened by increasing landfill age and demineralization, thereby facilitating the dechlorination of pentachlorophenol (PCP). The HLA molecules started to polymerize aromatic macromolecules during landfilling, leading to an increase in ETC and dechlorination capacities. Macromolecular HLA were dissociated to smaller molecules and exposed more aromatic and carboxyl groups when separated from minerals, which enhanced the ETC and the dechlorination abilities of the HLA. Microbial-mediated dechlorination was an effective way to degrade PCP, and almost 80% of the PCP was transformed after 40 days of demineralized HLA and Shewanella oneidensis MR-1 incubation. The demineralization and aging further facilitated the microbial-mediated PCP dechlorination. The findings provide a scientific base for improving in-situ bioremediation of chlorinated compound-contaminated soils using freshly synthesized HLA.
Mostrar más [+] Menos [-]Biouptake, toxicity and biotransformation of triclosan in diatom Cymbella sp. and the influence of humic acid Texto completo
2018
Ding, Tengda | Lin, Kunde | Bao, Lianjun | Yang, Mengting | Li, Juying | Yang, Bo | Gan, Jay
Triclosan is one of the most frequently detected emerging contaminants in aquatic environment. In this study, we investigated the biouptake, toxicity and biotransformation of triclosan in freshwater algae Cymbella sp. The influence of humic acid, as a representative of dissolved organic matter, was also explored. Results from this study showed that triclosan was toxic to Cymbella sp. with 72 h EC₅₀ of 324.9 μg L⁻¹. Humic acid significantly reduced the toxicity and accumulation of triclosan in Cymbella sp. SEM analysis showed that Cymbella sp. were enormously damaged under 1 mg L⁻¹ triclosan exposure and repaired after the addition of 20 mg L⁻¹ humic acid. Triclosan can be significantly taken up by Cymbella sp. The toxicity of triclosan is related to bioaccumulated triclosan as the algal cell numbers decreased when intracellular triclosan increased. A total of 11 metabolites were identified in diatom cells and degradation pathways are proposed. Hydroxylation, methylation, dechlorination, amino acids conjunction and glucuronidation contributed to the transformative reactions of triclosan in Cymbella sp., producing biologically active products (e.g., methyl triclosan) and conjugation products (e.g., glucuronide or oxaloacetic acid conjugated triclosan), which may be included in the detoxification mechanism of triclosan.
Mostrar más [+] Menos [-]The ecotoxic potential of a new zero-valent iron nanomaterial, designed for the elimination of halogenated pollutants, and its effect on reductive dechlorinating microbial communities Texto completo
2016
Schiwy, Andreas | Maes, Hanna M. | Koske, Daniel | Flecken, Mirkko | Schmidt, Kathrin R. | Schell, Heico | Tiehm, Andreas | Kamptner, Andre | Thümmler, Silke | Stanjek, H. (Helge) | Heggen, Marc | Dunin-Borkowski, Rafal E. | Braun, Jürgen | Schäffer, Andreas | Hollert, Henner
The purpose of this study was to assess the ecotoxic potential of a new zero-valent iron nanomaterial produced for the elimination of chlorinated pollutants at contaminated sites. Abiotic dechlorination through the newly developed nanoscale zero-valent iron material and its effects on dechlorinating bacteria were investigated in anaerobic batch and column experiments. The aged, i.e. oxidized, iron material was characterization with dynamic light scattering, transmission electron microscopy and energy dispersive x-ray analysis, x-ray diffractometry and cell-free reactive oxygen measurements. Furthermore, it was evaluated in aerobic ecotoxicological test systems with algae, crustacean, and fish, and also applied in a mechanism specific test for mutagenicity. The anaerobic column experiments showed co-occurrence of abiotic and biological dechlorination of the common groundwater contaminant perchloroethene. No prolonged toxicity of the nanomaterial (measured for up to 300 days) towards the investigated dechlorinating microorganism was observed. The nanomaterial has a flake like appearance and an inhomogeneous size distribution. The toxicity to crustacean and fish was calculated and the obtained EC50 values were 163 mg/L and 458 mg/L, respectively. The nanomaterial showed no mutagenicity. It physically interacted with algae, which had implications for further testing and the evaluation of the results. Thus, the newly developed iron nanomaterial was slightly toxic in its reduced state but no prolonged toxicity was recorded. The aquatic tests revealed a low toxicity with EC50 values ≥ 163 mg/L. These concentrations are unlikely to be reached in the aquatic environment. Hence, this nanomaterial is probably of no environmental concern not prohibiting its application for groundwater remediation.
Mostrar más [+] Menos [-]Enriching for microbial reductive dechlorination of polychlorinated dibenzo-p-dioxins and dibenzofurans Texto completo
2014
Liu, Hui | Park, Joong-Wook | Häggblom, Max M.
Anaerobic enrichment cultures derived from contaminated Kymijoki River sediments dechlorinated 1,2,3,4-tetrachlorodibenzofuran (1,2,3,4-tetra-CDF), octachlorodibenzofuran (octa-CDF) and 1,2,3,4-tetrachlorodibenzo-p-dioxin (1,2,3,4-tetra-CDD). 1,2,3,4-tetra-CDF was dechlorinated via 1,2,3-, 2,3,4-, and 1,3,4/1,2,4-tri-CDFs to 1,3-, 2,3-, and 2,4-di-CDFs and finally to 4-mono-CDF. The dechlorination rate of 1,2,3,4-tetra-CDF was generally slower than that of 1,2,3,4-tetra-CDD. The rate and extent of 1,2,3,4-tetra-CDD dechlorination was enhanced by addition of pentachloronitrobenzene (PCNB) as a co-substrate. Dechlorination of spiked octa-CDF was observed with the production of hepta-, hexa-, penta- and tetra-CDFs over 6 months. Two major phylotypes of the Chloroflexi community showed an increase, one of which was identical to the Dehalococcoides mccartyi Pinellas subgroup. A set of twelve putative reductive dehalogenase (rdh) genes increased in abundance with addition of 1,2,3,4-tetra-CDF, 1,2,3,4-tetra-CDD and/or PCNB. This information will aid in understanding how indigenous microbial communities impact the fate of PCDFs and in developing strategies for bioremediation of PCDD/F contaminated sediments.
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