ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Guiping Liu,Kai Chen,Zhiming Wu,Yanhan Ji,Lianghua Lu,Songmeng Liu,Zhi-Ling Li,Rong Ji,Shuang-Jiang Liu,Jiandong Jiang,Wenjing Qiao
Tetrabromobisphenol A (TBBPA), a widely used brominated flame retardant in electronics manufacturing, has caused global contamination due to improper e-waste disposal. Its persistence, bioaccumulation, and potential carcinogenicity drive studies of its transformation and underlying (a)biotic interactions. This study achieved an anaerobic enrichment culture capable of reductively dehalogenating TBBPA to the more bioavailable bisphenol A. 16S rRNA gene amplicon sequencing and quantitative PCR confirmed that successive dehalogenation of four bromide ions from TBBPA was coupled with the growth of both Dehalobacter sp. and Dehalococcoides sp. with growth yields of 5.0 ± 0.4 × 108 and 8.6 ± 4.6 × 108 cells per μmol Br– released (N = 3), respectively. TBBPA dehalogenation was facilitated by solid humin and reduced humin, which possessed the highest organic radical signal intensity and reducing groups −NH2, and maintained the highest dehalogenation rate and dehalogenator copies. Genome-centric metatranscriptomic analyses revealed upregulated putative TBBPA-dehalogenating rdhA (reductive dehalogenase) genes with humin amendment, cprA-like Dhb_rdhA1 gene in Dehalobacter species, and Dhc_rdhA1/Dhc_rdhA2 genes in Dehalococcoides species. The upregulated genes of lactate fermentation, de novo corrinoid biosynthesis, and extracellular electron transport in the humin amended treatment also stimulated TBBPA dehalogenation. This study provided a comprehensive understanding of humin-facilitated organohalide respiration.
研究领域:
环境微生物学
·
基因组学
·
生物修复
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Guiping Liu,Songmeng Liu,Jie Yang,Xiaoyang Zhang,Lianghua Lu,Hongxia Xu,Shujun Ye,Jichun Wu,Jiandong Jiang,Wenjing Qiao
Tetrabromobisphenol A (TBBPA), a common brominated flame retardant and a notorious pollutant in anaerobic environments, resists aerobic degradation but can undergo reductive dehalogenation to produce bisphenol A (BPA), an endocrine disruptor . Conversely, BPA is resistant to anaerobic biodegradation but susceptible to aerobic degradation. Microbial degradation of TBBPA via anoxic/oxic processes is scarcely documented. We established an anaerobic microcosm for TBBPA dehalogenation to BPA facilitated by humin. Dehalobacter species increased with a growth yield of 1.5 × 10 8 cells per μmol Br - released, suggesting their role in TBBPA dehalogenation. We innovatively achieved complete and sustainable biodegradation of TBBPA in sand/soil columns columns, synergizing TBBPA reductive dehalogenation by anaerobic functional microbiota and BPA aerobic oxidation by Sphingomonas sp. strain TTNP3. Over 42 days, 95.11 % of the injected TBBPA in three batches was debrominated to BPA. Following injection of strain TTNP3 cells, 85.57 % of BPA was aerobically degraded. Aerobic BPA degradation column experiments also indicated that aeration and cell colonization significantly increased degradation rates. This treatment strategy provides valuable technical insights for complete TBBPA biodegradation and analogous contaminants.
研究领域:
环境科学
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微生物学
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生物修复
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2016
·
IF 5.991
Wenhai Chu,Xin Li,Tom Bond,Naiyun Gao,Xu Bin,Qiongfang Wang,Shunke Ding
The haloacetamides (HAcAms), an emerging class of nitrogen-containing disinfection byproducts (N-DBPs), are highly cytotoxic and genotoxic, and typically occur in treated drinking waters at low μg/L concentrations. Since many drinking distribution and storage systems contain unlined cast iron and copper pipes, reactions of HAcAms with zero-valent iron (ZVI) and metallic copper (Cu) may play a role in determining their fate. Moreover, ZVI and/or Cu are potentially effective HAcAm treatment technologies in drinking water supply and storage systems. This study reports that ZVI alone reduces trichloroacetamide (TCAcAm) to sequentially form dichloroacetamide (DCAcAm) and then monochloroacetamide (MCAcAm), whereas Cu alone does not impact HAcAm concentrations. The addition of Cu to ZVI significantly improved the removal of HAcAms, relative to ZVI alone. TCAcAm and their reduction products (DCAcAm and MCAcAm) were all decreased to below detection limits at a molar ratio of ZVI/Cu of 1:1 after 24 h reaction (ZVI/TCAcAm = 0.18 M/5.30 μM). TCAcAm reduction increased with the decreasing pH from 8.0 to 5.0, but values from an integrated toxic risk assessment were minimised at pH 7.0, due to limited removal MCAcAm under weak acid conditions (pH = 5.0 and 6.0). Higher temperatures (40 °C) promoted the reductive dehalogenation of HAcAms. Bromine was preferentially removed over chlorine, thus brominated HAcAms were more easily reduced than chlorinated HAcAms by ZVI/Cu. Although tribromoacetamide was more easily reduced than TCAcAm during ZVI/Cu reduction, treatment of tribromoacetamide resulted in a higher integrated toxicity risk than TCAcAm, due to the formation of monobromoacetamide (MBAcAm).
研究领域:
环境科学
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公共卫生
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF BIOTECHNOLOGY
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2015
·
IF 2.871
Nan-Wei Wan,Zhi-Qiang Liu,Feng Xue,Yu-Guo Zheng
A halohydrin dehalogenase (HHDH-PL) from Parvibaculum lavamentivorans DS-1 was characterized and applied to determine azide and cyanide in the water. In this methodology, HHDH-PL catalysed azide and cyanide to react with butylene oxide and form corresponding β-substituted alcohols 1-azidobutan-2-ol (ABO) and 3-hydroxypentanenitrile (HPN) that could be quantitatively detected by gas chromatograph. The detection calibration curves for azide ( R 2 = 0.997) and cyanide ( R 2 = 0.995) were linear and the lower limits of detection for azide and cyanide were 0.1 and 0.3 mM, respectively. Several other nucleophiles were identified having no effect on the analysis of azide and cyanide, excepting nitrite which influenced the detection of cyanide. This was the first report of a biological method to determine the inorganic azide and cyanide by converting them to the measurable organics.
研究领域:
生物化学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2016
·
IF 3.299
Xiaodan Zhao,Jun Ma,Jin Jiang,Yuhuan Bao,Huiling Liu
Synergistic enhancement of phenols and anilines removal was investigated in permanganate oxidation in the presence of multi-walled carbon nanotubes (CNTs). Then the attendant dehalogenation was explored for bromophenols and bromoanilines from the perspective of dehalogenation number (DN). Permanganate decay and total manganese concentration decrease in the presence of CNTs indicates considerable formation of manganese dioxide (MnO 2 ) on carbon surface. The CNTs-enhanced phenol degradation is more favorable under lower pH, confirming that the generation of MnO 2 induced by the reaction between permanganate and CNTs enhances the phenol oxidation by permanganate. The first order rate constants of respective bromophenols and bromoanilines suggest the synergistic enhancement of CNTs and permanganate in removing these micropollutants. Bromide release experiments clearly demonstrate that the subsequent dehalogenation accompanying the oxidation of bromophenols and bromoanilines is significant for permanganate oxidation in the absence/presence of CNTs. Dehalogenation by permanganate follows the order of 4-bromophenol > 2-bromophenol > 3-bromophenol and 4-bromoaniline > 2-bromoaniline > 3-bromoaniline, respectively. Higher DN values in the presence of CNTs indicate a reduced dehalogenation. In real water application, permanganate in the presence of CNTs could effectively remove 4-bromoaniline with a maximum removal efficiency of ∼95% and a bromide release of 2 μM.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2024
·
IF 8.2
Shasha Fang,Yue Geng,Lu Wang,Jun Zeng,Shimin Zhang,Yucheng Wu,Xiangui Lin
Polybrominated diphenyl ethers (PBDEs) are persistent pollutants that may undergo microbial-mediated debromination in anoxic environments, where diverse anaerobic microbes such as methanogenic archaea co-exist. However, current understanding of the relations between PBDE pollution and methanogenic process is far from complete. To address this knowledge gap, a series of anaerobic soil microcosms were established. BDE-47 (2, 2′, 4, 4′-tetrabromodiphenyl ether) was selected as a model pollutant, and electron donors were supplied to stimulate the activity of anaerobes . Debromination and methane production were monitored during the 12 weeks incubation, while obligate organohalide-respiring bacteria (OHRBs), methanogenic, and the total bacterial communities were examined at week 7 and 12. The results demonstrated slow debromination of BDE-47 in all microcosms, with considerable growth of Dehalococcoides and Dehalogenimonas over the incubation observed in most BDE-47 spiked treatments. In addition, the accumulation of intermediate metabolites positively correlated with the abundance of Dehalogenimonas at week 7, suggesting potential role of these OHRBs in debromination. Methanosarcinaceae were identified as the primary methanogenic archaea, and their abundance were correlated with the production of debrominated metabolites at week 7. Furthermore, it was observed for the first time that BDE-47 considerably enhanced methane production and increased the abundance of mcrA genes, highlighting the potential effects of PBDE pollution on climate change. This might be related to the inhibition of reductive N- and S-transforming microbes, as revealed by the quantitative microbial element cycling (QMEC) analysis. Overall, our findings shed light on the intricate interactions between PBDE and methanogenic processes, and contribute to a better understanding of the environmental fate and ecological implication of PBDE under anaerobic settings.
研究领域:
环境科学
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微生物学
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生态学
·
土壤学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
He Jiang,Haoliang Wei,Xinkai Li,Yijun Zhang,Tingjiang Lu,Feili Li,Shuang Song,Yan Yu,Meilan Pan,Weiting Yu
The widespread discharge of halogenated organic pollutants (HOPs) in wastewater brings significant risks to the environment and human health due to potent high toxicity, antibacterial activity, and strong biodegradation resistance. Adsorbed atomic hydrogen (H* ads )-mediated electrocatalytic hydrodehalogenation (EHDH) has been recognized as an efficient strategy for HOPs removal through selectively breaking carbon-halogen bonds. In this work atomic Pd uniformly anchored on molybdenum disulfide (denoted as Pd-MoS 2 ) was synthesized through a facile hydrothermal method and found with state-of-the-art specific activity in florfenicol (FLO) removal via the H* ads -mediated EHDH process. Pd-MoS 2 completely dehalogenated (∼100 %) FLO within 30 min at a rate constant of 0.15 min −1 , which was 6.0, 6.5 and 33.1 times the value of MoS 2 , Pd/C and carbon paper samples, respectively. Notably, the toxicity of the wastewater was reduced to 1/6 of its original value after the treatment. Moreover, Pd-MoS 2 presented superior catalytic stability in five successive cycles. Furthermore, Pd-MoS 2 was also robust in complex water environment with practical applicability for industrial wastewater treatment. A dual-active-center mechanism with enhanced H* ads production capacity and the improved H* ads utilization efficiency was contributed to the increased EHDH activity on Pd-MoS 2 .
研究领域:
环境科学
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材料科学
·
化学工程
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DOI
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Yunxia Zu,Zhiling Li,Zimeng Zhang,Xueqi Chen,Bin Wu,Shih-Hsin Ho,Aijie Wang
Biological iron reduction and reductive dehalogenation occur in similar ecological environments, however, how Fe(III)/Fe(II) redox cycles impact the microbial dehalogenation processes remains controversial. In this study, the favorable microbial reductive dechlorination activity has been widely observed in iron-rich river sediments by national sampling, with the dechlorination efficiency showing a positive correlation with the concentration of Fe(III). Microcosm experiments demonstrated that the addition of nano-hematite resulted in a maximum increase of 2.16 times in the dechlorination rate constant ( k ) for 2,4,6-trichlorophenol, achieved via synergistic interactions with Fe(III) reduction. Multi-tools, including transcriptomic analyses, revealed that the addition of nano-hematite enhanced the process of Fe(III) reduction by upregulating genes associated with extracellular electron transfer (e.g., CYC, pliM ) and conductive biofilm formation (e.g., livH, secY, wza ). This synergistic Fe(III) reduction further facilitated intracellular carbon metabolism, energy production, and reductive dechlorination, as confirmed by the upregulated functional genes identified through transcriptomics and RT- q PCR. The discovery of the novel phenomenon involving synergistic Fe(III) reduction and dehalogenation broadens our understanding of the biochemical cycling of organohalides (e.g., chlorinated phenols) in iron-rich environment, and provides a feasible strategy for improving biodehalogenation through the regulation of carbon and electron flow at sites contaminated with organohalides.
研究领域:
环境微生物学
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生物地球化学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Mingjie Huang,Yi Han,Wei Xiang,Chen Wang,Juan Mao,Tao Zhou,Xiaohui Wu,Han-Qing Yu
The nucleophilic superoxide radical (O2•–)-based dehalogenation reaction shows great potential to degrade the toxic halogenated organic compounds (HOCs). But such an O2•–-mediated reductive reaction often suffers from the competition of the secondary oxidative species (e.g., •OH), leading to inferior electron efficiency and possible disinfection byproduct formation. Here, an O2•–-dominant ultrafast dehalogenation system is developed via molecular O2 activation by the oxygen vacancy (OV)-rich CuO nanoparticles (nCuO). The nCuO delivers a remarkable dechlorination rate constant of 3.92 × 10–2 L min–1 m–2 for 2,4-dichlorophenol, much higher than that of the conventional zerovalent (bi)metals. The absorbed O2 on the nCuO surface is exclusively responsible for O2•– generation, and its reactivity increases with the elevated OV content because of the enhanced orbital hybridization between the O p- and Cu d-orbitals. More importantly, the ubiquitous carbonate species firmly bound to the surface OVs block the formation of the secondary oxidative species via H2O2 activation, assuring the dominant role of the in situ generated O2•– for the selective HOC dehalogenation. The carbonate-deactivated OVs of the nCuO can be feasibly recovered via air annealing for sustainable dehalogenation. This work provides a new opportunity for selective O2•– generation via interfacial defect engineering for dehalogenation and other environmental applications.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2024
·
IF 7.4
Lan-Ying Liu,Min-Hua Cui,Shi-Ming Niu,Xue-Dong Zhang,Xin-Hui Li,Wo-Long Wang,He Liu,Guo-Shuai Liu,Ai-Jie Wang
In this study, we synthesized a phosphorus-coordinated Pd@MXene catalyst to address the drawbacks associated with high noble metal usage, susceptibility to poisoning, and stability issues in the electrocatalytic hydrodehalogenation (EHDC) of recalcitrant halogenated pollutants. The phosphorus-coordinated Pd@MXene exhibited an EHDC performance comparable to that of the benchmark electrode (Pd@MX/CC) when tested on the model pollutant diclofenac (DCF). Notably, the phosphorus-coordinated Pd electrode demonstrated an 80% reduction in Pd usage and a 3.9-fold increase in Pd utilization efficiency. This improved performance was consistent across a wide range of pH values (pH 3, 7, and 11) and was sustained over 10 reaction cycles for the removal of DCF. Furthermore, the enhanced catalytic activity of the phosphorus-coordinated Pd electrode was achieved in the EHDC of various halogenated compounds. Importantly, the electrode exhibited a favorable tolerance to inorganic ions during the EHDC process. Density functional theory (DFT) calculations provided insights into the electronic configuration regulation of phosphorus-coordinated Pd@MXene, optimizing binding energies for H* and dechlorinated intermediates. The reported promotion effect of halogenated pollutants degradation by the phosphorus-coordination approach offers new insights into efficient EHDC systems toward water purification.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
MOLECULES
·
2016
·Vol. 21
·期 7
·895
·
IF 2.465
Hui Jian,Yingwu Wang,Yan Bai,Rong Li,Renjun Gao
Formylglycine-generating enzymes can selectively recognize and oxidize cysteine residues within the sulfatase sub motif at the terminus of proteins to form aldehyde-bearing formylglycine (FGly) residues, and are normally used in protein labeling. In this study, an aldehyde tag was introduced to proteins using formylglycine-generating enzymes encoded by a reconstructed set of the pET28a plasmid system for enzyme immobilization. The haloacid dehalogenase ST2570 fromSulfolobus tokodaiiwas used as a model enzyme. The C-terminal aldehyde-tagged ST2570 (ST2570CQ) exhibited significant enzymological properties, such as new free aldehyde groups, a high level of protein expression and improved enzyme activity. SBA-15 has widely been used as an immobilization support for its large surface and excellent thermal and chemical stability. It was functionalized with amino groups by aminopropyltriethoxysilane. The C-terminal aldehyde-tagged ST2570 was immobilized to SBA-15 by covalent binding. The site-specific immobilization of ST2570 avoided the chemical denaturation that occurs in general covalent immobilization and resulted in better fastening compared to physical adsorption. The site-specific immobilized ST2570 showed 3-fold higher thermal stability, 1.2-fold higher catalytic ability and improved operational stability than free ST2570. The site-specific immobilized ST2570 retained 60% of its original activity after seven cycles of batch operation, and it was superior to the ST2570 immobilized to SBA-15 by physical adsorption, which loses 40% of its original activity when used for the second time. It is remarkable that the site-specific immobilized ST2570 still retained 100% of its original activity after 10 cycles of reuse in the semi-continuous flow reactor. Overall, these results provide support for the industrial-scale production and application of site-specific, covalently immobilized ST2570.
研究领域:
生物化学
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酶工程
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材料科学
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DOI
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Wendi Guo,Zehui Sun,Meng-Jiao Xu,Kaizhi Wang,Mugeng Chen,Conglin Zhu,Heyong He,Yong-Mei Liu,Yong Cao
The efficient and environmentally friendly removal of halogen substituents from organic substances is crucial for reducing the ecological and health hazards posed by persistent halogenated compounds. In this regard, we introduce CoN3P1@NP-PC, a novel asymmetric CoN3P1 single-atom catalyst, which demonstrates outstanding efficiency in transfer hydrodehalogenation (HDH) using just two equivalents of HCOONH4 as a benign and effective reducing agent. This catalyst was synthesized through a simple post-implantation method, capitalizing the high porosity and large surface area of ZIF-8 precursors. Extensive characterization via a range of spectroscopic and microscopic techniques confirmed CoN3P1@NP-PC's superior atomic dispersion and asymmetric structural integrity, which was more favourable for HCOONH4 activation allowing facile generation of hydrogen radical along with electron transfer. In our comprehensive evaluation, CoN3P1@ NP-PC displayed outstanding versatility for transformation of a diverse array of halogenated substrates, efficiently processing compounds with varied functional groups and complex molecular structures. Notably, CoN3P1@NP-PC proved particularly effective in breaking down brominated flame retardants such as 2,4,6-tribromophenol and tetrabromobisphenol A, reinforcing its potential as a powerful tool for ecological restoration and pollution control.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）