CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jiating Liu,Peizeng Yang,Yuefei Ji,Junhe Lu
Sulfate radical (SO 4 •- )-based advanced oxidation processes (SR-AOPs) show great potential in the elimination of organic pollutants in wastewater treatment and groundwater remediation . Tetrabromobisphenol S (TBBPS) as an emerging contaminant can be effectively degraded in SR-AOPs. However, the present study found that SO 4 •- also reacted with ammonium (NH 4 + ), a ubiquitous inorganic nitrogen species in aquatic environments, thus markedly affected the rates and pathways of TBBPS degradation in SR-AOPs. TBBPS underwent β-scission and debromination upon SO 4 •- attack, leading to various transformation products . The released bromide (Br - ) underwent further oxidation by SO 4 •- to form free bromine which reacted with certain TBBPS intermediates, generating disinfection byproducts (DBPs). When NH 4 + was present in such system, the abatement of TBBPS was apparently suppressed. Meanwhile, NH 4 + was oxidized by SO 4 •- to nitrogen dioxide radical (NO 2 • ) which coupled with certain radical intermediates of TBBPS oxidation, yielding nitrophenolic products including 2,6-dibromo-4-nitrophenol (DBNP) and mono-nitro substituted TBBPS. When 10 μM TBBPS was treated by heat activated peroxydisulfate with 1 mM NH 4 + , the molar yield of DBNP reached 22% in 2 h. More importantly, NH 4 + scavenged the in situ formed free bromine to form monobromamine (NH 2 Br), decreasing regulated DBPs formation but leading to highly toxic dibromoacetonitrile (DBAN). This study broadens the understanding of interactions between the transformation of halogens and NH 4 + during SO 4 •- oxidation. It also reveals the potential environmental risks when SR-AOPs are employed for the organohalogen pollutants degradation in realistic environments where NH 4 + is present.
研究领域:
环境科学
·
水处理工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Peizeng Yang,Jiating Liu,Gregory V. Korshin,Yuefei Ji,Junhe Lu
Tetrabromobisphenol S (TBBPS) is a brominated flame retardant and a contaminant of emerging concern. Several studies found that sulfate radical (SO4•–) oxidation is effective to degrade TBBPS. Here, we demonstrate that the presence of nitrite (NO2–) at environmentally relevant levels causes dramatic changes in the kinetics and pathways of TBBPS degradation by SO4•–. Initially, NO2– suppresses the reaction by competing with TBBPS for SO4•–. At the same time, SO4•– oxidizes NO2– to form nitrogen dioxide radicals (NO2•), which actively react with some key TBBPS degradation intermediates, thus greatly altering the transformation pathway. As a result, 2,6-dibromo-4-nitrophenol (DBNP) becomes the primary TBBPS product. As TBBPS undergoes degradation, the released bromide (Br–) is oxidized by SO4•– to form bromine radicals and free bromine. These reactive bromine species immediately combine with NO2• or NO2– to form nitryl bromide (BrNO2) that in turn attacks the parent TBBPS, resulting in its accelerated degradation and increased formation of toxic nitrophenolic byproducts. These results show that nitryl halides (e.g., BrNO2 or ClNO2) are likely formed yet inadequately recognized when SO4•– is applied to remediate halogenated pollutants in the subsurface environment where NO2– is ubiquitously found. These insights further underscore the potential risks of the application of SO4•– oxidation for the remediation of halogenated compounds in realistic environmental conditions.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
PubMed
高影响因子
MICROCHEMICAL JOURNAL
·
2019
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IF 3.206
Kwabena Agyarko Sarpong,Kun Zhang,Yu Luan,Yunfei Cao,Wanzhen Xu
Tetrabromobisphenol-S (TBBPS) is a Brominated Flame Retardants (BFRs). TBBPS in trace quantities is lethal and do not only alter the normal performance of the endocrine system but can directly or indirectly provoke hepatoxicity and carcinogenic diseases. Herein, we fabricate a facile electrochemical sensor and investigate its application towards the determination of TBBPS through imprinting technique. TBBPS imprinting was carried out in the presence of methacrylic acid (MAA) and 4-aminothiophenol (4-ATP) functional monomers (DiM) over gold nanoparticles (AuNPs) modified carbon paste electrode (CPE). Transmission electron microscopy (TEM) was used to characterize the imprinted sensor. Performance was thoroughly investigated using both cyclic voltammetry (CV) and differential pulse voltammetry (DPV). The proposed sensor showed detection behavior towards TBBPS in standard solutions with different concentrations range of 0.1 nM-10 nM and with a detection limit of 0.029 nM. The developed MIP(DiM)@AuNPs/CPE sensor had enhanced recognition capacity compared to MIP electrochemical sensors developed with a mono functional monomer (MIP(MoM)@AuNPs/CPE) and non-imprinted sensors. In addition, the low cost; easier preparation; excellent stability; and good selectivity of MIP(DiM)@AuNPs/CPE electrochemical sensor makes it an attractive alternative to high instrumentation detection techniques.
研究领域:
环境科学
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分析化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
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IF 7.4
Hui Li,Xinlei Ren,Wenxue Pan,Shiting Zhu,Jin Zhang,Zhiyuan Yang,Liu Qian,Yueying Wang,Yujing Huang,Lin Guo,Minghui Xiang
The reasonable control of the structure of metal–organic frameworks (MOFs) is a promising strategy for improving their peroxymonosulfate (PMS) activation activity. In this study, ZIF-67 @ZIF-8 was used as a template to prepare bimetallic core–shell Co-Fe@NC via Fe doping and high-temperature carbonization . Co-Fe@NC maintained the core–shell structure of the original MOF, in which cobalt was uniformly distributed in the nitrogen-doped graphite carbon skeleton and the surface of the graphite carbon skeleton was covered with iron. With the synergistic effect of the nitrogen-doped graphite carbon skeleton, iron, and cobalt, 100% of tetrabromobisphenol S (TBBPS) was removed in 60 min with k obs = 0.062 min −1 in Co-Fe@NC-0.2/PMS system. The addition of iron increased the graphitization degree with I D /I G value increased from 0.98 (Co@NC) to 1.034 (Co-Fe@NC-0.2) and electron transfer rate of the carbon skeleton. Besides, the Co leaching was effectively attenuated from 1.86 mg/L(Co@NC) to 0.78 mg/L (Co-Fe@NC-0.2) by the core-shell structure and bimetal strategy. Both O 2 · - and 1 O 2 contributed to the degradation of TBBPS according to quenching experiments. TBBPS was deeply degraded into small-molecule compounds through three degradation pathways by the Co-Fe@NC-0.2/PMS system. This study provides a new strategy for designing highly efficient bimetal–carbon composites for environmental remediation.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2024
·
IF 0
Qin Chao,Wu Junxue,Lu Xinyu,Gu Chenggang,Guo Yang,Hu Guanjiu,Chen Min,Xia Kang,Wang Hui,Xie Mingjie
The widespread occurrence of emerging brominated flame retardant tetrabromobisphenol S (TBBPS) has become a major environmental concern. In this study, a nanoscale zero-valent iron (nZVI) impregnated organic montmorillonite composite (nZVI-OMT) was successfully prepared and utilized to degrade TBBPS in aqueous solution. The results show that the nZVI-OMT composite was very stable and reusable as the nZVI was well dispersed on the organic montmorillonite. Organic montmorillonite clay layers provide a strong support, facilitate well dispersion of the nZVI chains, and accelerate the overall TBBPS transformation with a degradation rate constant 5.5 times higher than that of the original nZVI. Four major intermediates, including tribromobisphenol S (tri-BBPS), dibromobisphenol S (di-BBPS), bromobisphenol S (BBPS), and bisphenol S (BPS), were detected by high-resolution mass spectrometry (HRMS), indicating sequential reductive debromination of TBBPS mediated by nZVI-OMT. The effective elimination of acute ecotoxicity predicted by toxicity analysis also suggests that the debromination process is a safe and viable option for the treatment of TBBPS. Our results have shown for the first time that TBBPS can be rapidly degraded by an nZVI-OMT composite, expanding the potential use of clay-supported nZVI composites as an environmentally friendly material for wastewater treatment and groundwater remediation.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Lu Wang,Yaqun Yu,Guoqiang Liu,Junhe Lu
Tetrabromobisphenol S (TBBPS), an emerging brominated flame retardant , can cause neurotoxic and cytotoxic effects to human physiology . In this study, the degradation of TBBPS in Co 2+ activated peroxymonosulfate (PMS) oxidation process was explored. In particular, brominated by-products formed during the degradation of the TBBPS were examined. It was found that TBBPS could be effectively removed in the Co 2+ /PMS oxidation process. The pseudo-first-order rate constants were 0.13 min −1 at 0.2 mM PMS and 0.5 μM Co 2+ initially. It appeared that TBBPS degradation occurred via and HO attacks, but played a dominant role. The presence of natural organic matter (NOM) greatly inhibited the transformation of the TBBPS, which can be explained by the scavenging of the radical species. β-Scission, debromination, and cross-coupling were identified as the main reaction pathways of TBBPS degradation in the Co 2+ /PMS system. Further oxidation and ring-opening of the intermediates generated brominated by-products including bromoform, monobromoacetic acid, and dibromoacetic acid. The formation of the brominated by-products increased gradually in approximately 48 h. But, the presence of NOM reduced the yields of the brominated -by-products. The findings of this study indicate that organic bromine contaminants can be effectively removed but lead to brominated by-products in the activated PMS oxidation process, which should be taken into consideration when -based oxidation technology is applied.
研究领域:
环境科学
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化学工程
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水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2016
·
IF 2.822
Fang Long,Jing Wang,Zhaohui Zhang,Liang Yan
A novel magnetic molecularly imprinted electrochemical sensor (MMIP-sensor) combined with magnetic molecularly imprinted solid-phase extraction (MMISPE) was constructed for rapid and sensitive detection of tetrabromobisphenol S (TBBPS) in water samples. The magnetic molecularly imprinted polymer based on magnetic graphene/multi-walled carbon nanotubes hybrid composite (MMIP/Gr-MWCNTs) was prepared as MMISPE sorbet to separate and enrich TBBPS from complex system. Adsorption results showed that the MMIP/Gr-MWCNTs possessed excellent selective adsorption toward TBBPS with a maximum adsorption capacity of 17.83 mg g − 1 . The magnetic imprinted sensor based on the magnetic Gr-MWCNTs composite modified electrode was prepared by electropolymerization of dopamine monomer . The high sensitivity of the MMIP-sensor was attributed to the large specific surface area and excellent electrical conductivity of the magnetic Gr-MWCNTs composites. The detection limit of the MIP-sensor toward TBBPS was calculated as 2.1 × 10 − 11 mol L − 1 (S/N = 3). Under the optimum conditions, the MISPE-MMIP-sensor combination system provided 10–12 fold preconcentration than that of MMIP-sensor alone determination. The MISPE-MMIP-sensor was successfully used for detection of TBBPS in drinking water , rain water , lake water and tap water with recoveries of 88.4–98.8%.
研究领域:
分析化学
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环境监测
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电化学传感
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分子印迹技术
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水处理
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污染物检测
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2022
·
IF 3.475
Lu Wang,Yaqun Yu,Guoqiang Liu,Baowei Hu,Junhe Lu
Brominated flame retardants (BFRs) are a group of contaminants of emerging environmental concern. In this study, systematic exploration was carried out to investigate the degradation of tetrabromobisphenol S (TBBPS), a typical emerging BFRs, by thermally activated persulfate (PDS) oxidation. The removal of 5.0 μM TBBPS was 100% after 60 min oxidation treatment under 60°C. Increasing the temperature or initial PDS concentration facilitated the degradation efficiency of TBBPS. The quenching test indicated that TBBPS degradation occurred via the attack of both sulphate radicals and hydroxyl radicals. Natural organic matter (NOM) decreased the removal rate, however, complete disappearance of TBBPS could still be obtained. Six intermediate products were formed during reactions between TBBPS and radicals. Transformation pathways including debromination, β-Scission, and cross-coupling were proposed. Brominated disinfection by-products (DBPs) in situ formed during the degradation of TBBPS were also investigated, such as bromoform and dibromoacetic acid. The presence of NOM reduced the formation rates of brominated DBPs. Results reveal that although thermo-activated PDS is a promising method for TBBPS-contaminated water, it can lead to potential brominated DBPs risks, which should be paid more attention to when SO4•−-based oxidation technology is applied.
研究领域:
环境科学
·
化学工程
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
TALANTA
·
2017
·
IF 4.162
Xuemei Wang,Pengfei Huang,Xiaomin Ma,Huan Wang,Xiaoquan Lu,Xinzhen Du
Novel magnetic mesoporous molecularly imprinted polymers (MMIPs) with core-shell structure were prepared by simple surface molecular imprinting polymerization using tetrabromobisphenol-S (TBBPS) as the template. The MMIPs-TBBPS were characterized by fourier-transform infrared spectrometry (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N 2 adsorption-desorption transmission, and vibrating sample magnetometry . The resultant MMIPs-TBBPS were successfully applied magnetic solid-phase extraction (MSPE) coupled with HPLC determination of TBBPS in spiked real water samples with recoveries of 77.8–88.9%. The adsorption experiments showed that the binding capacity of MMIPs-TBBPS to TBBPS and six structural analogs were significantly higher than that of the magnetic nonimprinted polymers (MNIPs). Meanwhile, the MMIPs-TBBPS possessed rapid binding affinity , excellent magnetic response, specific selectivity and high adsorption capacity toward TBBPS with a maximum adsorption capacity of 1626.8 µg g −1 . The analytical results indicate that the MMIPs-TBBPS are promising materials for selective separation and fast enrichment of TBBPS from complicated enviromental samples.
研究领域:
材料科学
·
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）