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CHEMOSPHERE · 2022 · IF 8.943

Mechanochemical remediation of the chlorinated compounds contaminated soil depending on the minerals inside-the most reasonable approach

Zhenzhen Yao,Xiaoman He,Qian Wang,Chao Wang,Qing Shi,Qiwu Zhang

This study explored a possible destruction of hexachlorobenzene (HCB) as example of persistent organic pollutants (POPs) as well as the dechlorination mechanism by directly using minerals in the soil, such as antigorite , talc and olivine. Compared with a stable quartz phase of SiO 2 , all three Mg silicate minerals demonstrated certain degrading capacity for HCB with different efficiency order as: antigorite > talc > olivine > SiO 2 at 2 h of milling time. Interestingly, olivine exhibited a better performance than antigorite at 4 h of milling time, giving destruction percentage of 92.7% over 89.0% even at high concentrated HCB up to 5% added. Raman and ESR characterizations of the ball milled sample with olivine indicated the formation of amorphous carbon and graphitic carbon, and the occurrence of free radicals was observed to play an important role in dechlorination and carbonization of HCB. The first identified effectiveness of directly using Mg silicate minerals, allowed no addition of active chemicals during the ball milling, therefore avoided the concern over extrinsic contaminations on the soil. Olivine was further utilized to deal with actual contaminated soil and showed unique advantages on application prospects.

CAS / MDL: 110-54-3
研究领域: 环境科学 · 化学
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CHEMOSPHERE · 2016 · IF 3.698

Enhanced biodegradation of triclosan by means of gamma irradiation

Shizong Wang,Yanan Yin,Jianlong Wang

Triclosan is an antimicrobial agent which has been frequently detected in the environment. In this paper, the biodegradation of triclosan after radiation-induced advanced oxidation was investigated. The results show that the removal efficiency of triclosan in the combined irradiation and biological treatment process ranged from 88% to 97%, depending on the absorbed dose, while it was only 54% in the single biological treatment process. The removal efficiency of total organic carbon (TOC) was in the range of 53.1%,−59.2% at dose of 1–5 kGy in the combined irradiation and biological treatment process. In comparison, the removal efficiency of TOC in the single biological treatment process was 24.5%, suggesting that irradiation can enhance the mineralization of triclosan. The dechlorination efficiency of triclosan ranged from 48.6% to 78.4% at dose of 1–5 kGy. The intermediates of triclosan degradation were tentatively identified by LC-MS analysis and the possible degradation pathway was proposed. Based on the above results, the combined irradiation and biological treatment process could be an alternative process for treating triclosan-containing wastewater.

研究领域: 环境科学 · 生物学
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WATER RESEARCH · 2025 · IF 12.4

Photodegradation of PCB-209 on suspended particles: Discrepancy in mechanism of direct dechlorination and active species-mediated indirect dechlorination reactions

Jianqiao Xu,Xinyuan Wei,Junyan Wei,Mengqiang He,Xiaolei Teng,Zunyao Wang,Ruijuan Qu

While the reaction mechanism of direct photochemical dechlorination has been extensively studied, significant knowledge gaps remain regarding the specific roles of reactive species in governing dechlorination pathways during indirect photodegradation. By integrating mass spectrometry analysis, probe experiments and theoretical calculations, we propose for the first time an indirect dechlorination reaction mechanism for PCB-209 involving active species commonly found in DOM photosensitive systems, which differs significantly from that of direct photodegradation. Due to the lower bond energy of the C Cl bond at the position opposite the carbon bridge, PCB-209 primarily yielded PCB-208 in direct dechlorination systems. However, our study revealed that active species ( 3 DOM*, •O 2 − and 1 O 2 ) can specifically weaken the meta-positioned C Cl bond at the carbon bridge through electron transfer and cycloaddition mechanisms, thereby fundamentally altering the regioselectivity of dechlorination. Remarkably, our results confirm the indirect degradation of PCB-209 through DOM photosensitization to form dechlorination products dominated by PCB-207, a previously unrecognized transformation pathway in natural photochemical processes. This study refines the mechanism of indirect dechlorination mediated by reactive species and provides a predictive framework for the environmental fate of halogenated pollutants in real complex environmental systems.

CAS / MDL: 2051-24-3 39635-31-9
研究领域: 环境科学 · 化学
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RSC Advances · 2016 ·Vol. 6 ·期 80 ·76867-76873 · IF 3.289

A mechanically synthesized SiO2–Fe metal matrix composite for effective dechlorination of aqueous 2-chlorophenol: the optimum of the preparation conditions

Yunfei Zhang,Bo Yang,Jinhong Fan,Luming Ma

In this study, abrasives-reinforced metal matrix composites (MMCs) with a microscale size synthesized by ball milling (BM) could achieve highly active and stable dechlorination efficiency for aqueous 2-chlorophenol (2-CP). The preparation process of this composite via BM was optimized to obtain a high degradation efficiency, especially for the effect of the abrasives including B4C, SiC, α-Al2O3, SiO2, Fe3O4 and Na2SO4. The results showed that the hardness of the abrasives in the Fe-based MMCs was closely related with their dechlorination performance. Subsequently, the optimal abrasive, i.e. SiO2 was further investigated for its proper milling conditions with zero-valent iron (ZVI) particles including optimal SiO2 size, SiO2 loading, milling time, and the dosage of the process control agent (PCA). Additionally, the influence of other metal categories including Al and Si was also investigated for dechlorination; and their low reaction efficiencies were closely related with their passivating film. Finally, the longevity test suggested that the decreased reactivity of the SiO2–Fe MMC during the storage in air could be recovered when consecutively used, mainly due to the promoting effects of the inherent structure of SiO2–Fe MMC with the Fe/C and Fe/SiO2 interfaces, as well as the effective regeneration of the reactive sites by continuous iron dissolution.

研究领域: 环境科学 · 材料科学
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Electrocatalytic dechlorination of aqueous trichloroacetic acid by Vitamin B12 modified iron electrode

Xiaoyan Ma,Sinong Huang,Yuhong Jin,Hang Jiang,Liangjie Tang,Yifei Wu,Yongjiong Ni,Shijun Zhu,Xueyan Li,Andrea M. Dietrich

Haloacetic acids (HAAs) are ubiquitously detected in drinking water and even persistent after boiling due to their stability and nonvolatility, which leads to risk exposure to human. To minimize the risk, HAAs removal through electrocatalytic reduction easily utilized in point-of-use household devices is proposed. Trichloroacetic acid (TCAA) as a typical target, was investigated using laboratory-prepared metal electrode modified with Vitamin B12 (VB12) by the drop coating method. The dechlorination performance and effects of influencing factors on the TCAA dechlorination by VB12/metal composite cathode were studied. Under the conditions of 10.0 mg VB12 loading and 7.0 mA/cm 2 current density, 92.9% TCAA removal efficiency was achieved within 5 h at 25 °C in neutral water solution. The degradation processes followed the first-order kinetic model. The results show that VB12/iron (Fe) electrode presented the superior electrocatalytic activity than VB12/aluminium and VB12/copper. The dechlorination efficiency of TCAA was promoted by higher VB12 loadings and current density; inhibited by alkaline condition and higher initial concentration of TCAA. The synergistic effect between atomic H* and VB12 occurred during the TCAA dechlorination process through the electron transfer . The proposed pathway elucidated that TCAA was dechlorinated to form dichloroacetic acid (DCAA) and monochloroacetic acid (MCAA), with acetic acid and chloride as ultimate products. This electrocatalysis system with VB12/Fe composite electrode exhibits high reaction efficiency, targeted dehalogenation, and environmental friendliness. This work is expected to provides a new way for the removal of halogenated DBPs at the tap and the safeguard drinking water for consumers.

研究领域: 环境科学 · 化学工程 · 水处理技术
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JOURNAL OF HAZARDOUS MATERIALS · 2019 · IF 7.65

Insight into chlorine evolution during hydrothermal carbonization of medical waste model

Dachao Ma,Qingge Feng,Boqing Chen,Xi Cheng,Kao Chen,Jiao Li

In order to reveal the chlorine behavior during hydrothermal carbonization (HTC) of medical waste, polyvinyl chloride and medical waste model (MW) were respectively treated by HTC at temperature ranging from 220 °C to 300 °C for 30 min. HTC products were characterized by Fourier Transform Infrared Spectrometer, X-ray Photoelectron Spectroscopy, etc. It is found that HTC can efficiently remove chlorine from both polyvinyl chloride and MW. The most dramatical dechlorination can be induced by HTC at around 240 °C. With HTC temperature increased, organic chlorine in HT-MW and solid product from polyvinyl chloride HTC (HT-PVC) is decreased. Interestingly, with 240 °C HTC, the organic chlorine of HT-MW was 15.30%, much lower than that of HT-PVC of 86.84%, indicating the cellulosic materials in MW can significantly boost the conversion of organic chlorine into inorganic form in HTC at 240 °C. While spherical particles assigned to HTC of cellulosic materials aggregate at the pores of polyvinyl chloride particle, trapping the release of chlorine into the liquid, consequently to lower dechlorination efficiency compared to that of polyvinyl chloride. Since the chlorine retain in the solid product was mainly in form of inorganic, further dechlorination is potential for MW by combining HTC with leaching/extracting.

CAS / MDL: 9004-34-6
研究领域: 环境科学 · 化学工程
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Simultaneous removal of triclosan and nitrate by a stable denitrifying microbial consortium

Shizong Wang,Jun Hu,Jianlong Wang

The co-existence of antibiotics and nitrate in common in the aquatic environment, so the simultaneous removal of antibiotics and nitrate is necessary, but still challenge. In this study, a stable denitrifying microbial consortium capable of degrading triclosan was isolated from a long-term operated denitrifying bioreactor used for biological nitrate removal. The microbial consortium consisted of Pseudomonas (93.47 %), Burkholderia (1.56 %) and Cupriavidus (1.17 %) based on high-throughout sequencing analysis. The denitrification efficiency was higher under anoxic condition than that under aerobic condition . However, the accumulation of nitrite was observed under anoxic condition, with maximal concentration of 10.2 mg/L. Triclosan had negative impact on denitrification under both aerobic and anoxic conditions. The pseudo first-order kinetic constant of denitrification was 0.0303 h −1 and 0.0468 h −1 under aerobic and anoxic conditions, respectively. Dechlorination of triclosan was observed under aerobic condition but not under anoxic condition. Hydroxylated-triclosan, 2,4-dichlorophenol and phenol were identified as intermediate products of triclosan degradation.

CAS / MDL: 3380-34-5
研究领域: 环境科学 · 微生物学
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CHEMOSPHERE · 2023 · IF 8.8

Degradation and dechlorination of trichloroacetic acid induced by an in situ 222 nm KrCl* excimer radiation

Jiaming Gan,Ting Zhu,Yizhan Zhang,Dailin Li,Ting Li,Min Zhao,ZengXia Zhao,Lei Wang

Since the coronavirus disease 2019 (COVID-19) pandemic epidemic, the excessive usage of chlorinated disinfectants raised the substantial risks of disinfection by-products (DBPs) exposure. While several technologies may remove the typical carcinogenic DBPs, trichloroacetic acid (TCAA), their application for continuous treatment is limited due to their complexity and expensive or hazardous inputs. In this study, degradation and dechlorination of TCAA induced by an in situ 222 nm KrCl* excimer radiation as well as role of oxygen in the reaction pathway were investigated. Quantum chemical calculation methods were used to help predict the reaction mechanism. Experimental results showed that UV irradiance increased with increasing input power and decreased when the input power exceeded 60 W. Decomposition and dechlorination were simultaneously achieved, where around 78% of TCAA (0.62 mM) can be eliminated and 78% dechlorination within 200 min. Dissolved oxygen showed little effect on the TCAA degradation but greatly boosted the dechlorination as it can additionally generate hydroxyl radical (•OH) in the reaction process. Computational results showed that under 222 nm irradiation, TCAA was excited from S 0 to S 1 state and then decayed by internal crossing process to T 1 state, and a reaction without potential energy barrier followed, resulting in the breaking of C–Cl bond and finally returning to S 0 state. Subsequent C–Cl bond cleavage occurred by a barrierless •OH insertion and HCl elimination (27.9 kcal/mol). Finally, the •OH attacked (14.6 kcal/mol) the intermediate byproducts, leading to complete dechlorination and decomposition. The KrCl* excimer radiation has obvious advantages in terms of energy efficiency compared to other competitive methods. These results provide insight into the mechanisms of TCAA dechlorination and decomposition under KrCl* excimer radiation, as well as important information for guiding research toward direct and indirect photolysis of halogenated DBPs.

研究领域: 环境科学 · 化学工程
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Response of 2,4,6-trichlorophenol-reducing biocathode to burial depth in constructed wetland sediments

Tianming Chen,Chao Zou,Fan Chen,Ye Yuan,Jingjing Pan,Qi Zhao,Mansi Wang,Liang Qiao,Haoyi Cheng,Cheng Ding,Aijie Wang

Biocathode systems could be used for in-situ bioremediation of chlorophenols (CPs) in constructed wetland (CW) sediments. However, little is known regarding whether or how cathode burial depths affect the dechlorination of CPs in sediments. Here, 2,4,6-trichlorophenol (2,4,6-TCP)-dechlorinating biocathode systems were constructed under a cathode potential of − 0.7 V (vs. a saturated calomel electrode, SCE) at three different cathode burial depths (5, 10, and 15 cm). The 2,4,6-TCP removal efficiency and average transformation rate with the biocathode increased by 21.46–36.86% and 14.63–34.88% compared to those in the non-electrode groups. Deeper cathode burial depths enhanced the 2,4,6-TCP dechlorination performance. Furthermore, the oxidation-reduction potential (ORP) of the sediment decreased with sediment depth and the applied potential created a more favorable redox environment for the enrichment of functional bacteria. Deeper cathode burial depths also promoted the selective enrichment of electro-active and dechlorinating bacteria (e.g., Bacillus and Dehalobacter , respectively). The biocathode thus served as the carrier, electron source , and regulator of functional bacteria to accelerate the transformation of 2,4,6-TCP (2,4,6-TCP → 2,4-dichlorophenol → 4-chlorophenol → phenol) in sediments. These results offer insights into the effects of cathode burial depth on 2,4,6-TCP dechlorination in sediments from a redox environment and microbial community structure standpoint.

研究领域: 环境科学 · 微生物学
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ENVIRONMENTAL RESEARCH · 2022 · IF 8.431

Effects of different cathodic potentials on performance, microbial community structure and function for bioelectrochemical-stimulated dechlorination of 2,4,6-trichlorophenol in sediments

Chao Zou,Mansi Wang,Yixin Chen,Yu Qin,Yun Zhao,Liang Qiao,Shasha Zhu,Tianming Chen,Ye Yuan

Bioelectrochemical systems with biocathodes constitute a promising means to enhance the biological dechlorination of 2,4,6-trichlorophenol (2,4,6-TCP) in constructed wetland (CW) sediments. However, the effect of different cathodic potentials on the structure and function of 2,4,6-TCP-reducing biocathode communities in CW sediments is largely unknown. Here, we evaluated the performance and microbial community structure of 2,4,6-TCP-reducing biocathode systems at different cathodic potentials (− 0.5, − 0.7, − 0.9, and − 1.1 V vs. saturated calomel electrode). The dechlorination efficiency of 2,4,6-TCP with the biocathode relatively increased by 16.02%–33.17% compared to that in the open circuit. The highest 2,4,6-TCP dechlorination efficiency (92.34 ± 0.86%) was observed at − 0.7 V in sediment, which may be due to the highest abundance of functional genera (e.g., Pseudomonas , Spirochaeta ) at − 0.7 V. Metagenomic analysis provided new insights into the metabolic potential of microorganisms in CW sediments and suggested possible 2,4,6-TCP conversion pathways in sediments. 2,4,6-TCP was gradually dechlorinated to form 4-chlorophenol, followed by a ring-opening step via the activities of chlorophenol reductive dehalogenase and oxygenase (e.g., cprA , tfdB ). Interestingly, micro-electrical stimulation enhanced the expression of chlorophenol reductive dehalogenase ( cprA ). Therefore, our findings at the molecular and gene expression levels provide insights into the effects of different cathodic potentials on the performance and community structure of 2,4,6-TCP-reducing biocathode systems in CW sediments.

研究领域: 环境科学 · 微生物学
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Journal of Environmental Chemical Engineering · 2024 · IF 7.4

Enhancing trichloroethylene dechlorination capacity by utilizing granular ceramic material derived from Fe0-carbon-kaolin nanocomposite as substrate filter

Jiayan Zhu,Lishan Zhang,Junyong Liu,Shan Zhong,Zengxian Wei,Pin Gao,Jinyou Shen

In this study, we present a novel approach to fabricate a granular ceramic material utilizing a composite of nano zero-valent iron (nZVI), carbon, and kaolin. The optimal mass ratio of the prepared material was kaolin, nZVI, activated carbon, and appropriate additives = 40%:40%:10%:10%. The resulting composite demonstrated microelectrolysis effects, enhancing its reactivity for pollutant removal. Activated carbon within the composite significantly increased the interlayer spacing of kaolin, and improved material performance. Furthermore, the addition of activated carbon proved effective in preventing the agglomeration of nZVI, and ensuring a stable and efficient pollutant removal process. The results of 40-day column experiments showed that nano iron-carbon-kaolin micro-electrolysis particles (NIMP) consistently demonstrated stable trichloroethane (TCE) removal with an average removal rate of 88.15 ± 3.24%. Batch experiments confirmed that the synthesized material can achieve complete dechlorination of TCE, which was consistent with density functional theory calculations. The developed material exhibited a robust soil structure and high reactivity for pollutant reduction, making it a promising substrate filler for efficiently degrading refractory organic pollutants. It holds great potential for applications in areas such as water treatment and soil remediation.

研究领域: 环境科学 · 材料科学
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BIORESOURCE TECHNOLOGY · 2018 · IF 5.807

Cathode potential regulation in a coupled bioelectrode-anaerobic sludge system for effective dechlorination of 2,4-dichloronitrobenzene

Linlin Chen,Junjie Shao,Hui Chen,Caiqin Wang,Xinyi Gao,Xiangyang Xu,Liang Zhu

For enhanced dechlorination of 2,4-dichloronitrobenzene (2,4-DClNB), a coupled microbial electrosynthesis-upflow anaerobic sludge reactor (MES-UASB) was established, and the effect of cathode potential on the performance of combined process was investigated in this study. Results showed that a higher dechlorination efficiency of 78.5 ± 6.1% was achieved in the coupled MES-UASB at −660 mV, and the degradation rate of 4-chloroaniline (4-ClAn) reached 4.61 mg·L −1 ·d −1 within 120 h at −660 mV of cathode potential in batch experiments. The results of Illumina sequencing indicated that the biocathode operated at a lower potential favored the enrichment of dechlorination-related microbes such as Dehalobacter , Dehalococcoides and Anaeromyxobacter both in granular sludge and cathode biofilm. It could be speculated that a lower cathode potential is more feasible for the dechlorination of 2,4-DClNB due to the enrichment of dechlorination-related microbes as well as the production of electrons with higher energy for long-distance electron transfer (LDET).

研究领域: 环境科学 · 微生物学
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