ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Chengxue Ma,Haijun Cheng,Ruixing Huang,Yijie Zou,Qiang He,Xiaoliu Huangfu,Jun Ma
The oxidation of thallium [Tl(I)] to Tl(III) by chlorine (HOCl) is an important process changing its removal performance in water treatment. However, the role of bromide (Br–), a common constituent in natural water, in the oxidation behavior of Tl(I) during chlorination remains unknown. Our results demonstrated that Br– was cycled and acted as a catalyst to enhance the kinetics of Tl(I) oxidation by HOCl over the pH range of 5.0–9.5. Different Tl(I) species (i.e., Tl+ and TlOH(aq)) and reactive bromine species (i.e., HOBr/BrO–, BrCl, Br2O, and BrOCl) were kinetically relevant to the enhanced oxidation of Tl(I). The oxidation by free bromine species became the dominant pathway even at a low Br– level of 50 μg/L for a chlorine dose of 2 mg of Cl2/L. It was found that the reactions of Tl+/BrCl, Tl+/BrOCl, and TlOH(aq)/HOBr dominated the kinetics of Tl(I) oxidation at pH < 6.0, pH 6.0–8.0, and pH > 8.0, respectively. The species-specific rate constants for Tl+ reacting with individual bromine species were determined and decreased in the order: BrCl > Br2 > BrOCl > Br2O > HOBr. Overall, the presented results refine our knowledge regarding the species-specific reactivity of TI(I) with bromine species and will be useful for further prediction of thallium mobility in chlorinated waters containing bromide.
研究领域:
环境科学
·
水处理化学
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DOI
高影响因子
CHEMOSPHERE
·
2019
·
IF 5.108
Qi Han,Wenyi Dong,Hongjie Wang,Hang Ma,Peng Liu,Yurong Gu,Hongkai Fan,Xin Song
This study systematically investigated the performance of ozonation on tetrabromobisphenol A (TBBPA) degradation under different ozone dosages (5.21–83.33 μmoL/L), initial solution pH (3.0–11.0) and temperatures (10–50 °C). At the same time, the generations of inorganic products (bromide ion and bromate) under different experimental conditions were evaluated and the organic products were also identified. Then, the possible mechanism was proposed and verified by the quantum chemical calculation. In addition, variations and controlling of the toxicity were also analyzed, including acute toxicity, chronic toxicity and genotoxicity. Ozonation was proved to be an efficient and promising technology for removing TBBPA from water. TBBPA of 1.84 μmoL/L could be completely degraded within 5 min under the ozone dosage of 41.67 μmoL/L in wide ranges of pH (3.0–11.0) and temperature (10–40 °C). During the degradation of TBBPA, over 65% of the average bromine ion was detected and nine products were identified. The proposed degradation pathways verified that TBBPA might undergo addition and stepwise oxidative debromination, the hydrogen extraction, and the deprotonation. The results of toxicity testing showed that ozonation could effectively control the acute and chronic toxicity of the water samples, although the toxicity increased in the initial reaction stage due to the accumulation of more toxic intermediates.
研究领域:
环境科学
·
化学工程
·
毒理学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2022
·
IF 4.198
Jun Ma,Qijie Zou,Chunhua Wang,Guangwei Yin,Fangyi Li
Herein, we report a base promoted dibromination of enamides using CBr4 as a bromine source to provide expedient access to β,β-dibrominated secondary enamides. Preliminary synthetic application study shows that these novel products can be readily transformed to 5-Br oxazoles via Cu(I) catalyzed intramolecular cyclization in good yields.
研究领域:
有机化学
·
合成化学
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DOI
PubMed
高影响因子
ACS Nano
·
2021
·
IF 15.881
Xinliang Li,Na Li,Zhaodong Huang,Ze Chen,Yuwei Zhao,Guojin Liang,Qi Yang,Mian Li,Qing Huang,Binbin Dong,Jun Fan,Chunyi Zhi
With fluidity and dangerous corrosiveness, liquid insulating bromine elemental (Br2) can hardly be confined by traditional conductive carriers (mainly carbon materials) for efficient redox without shuttle behavior. Thus, stationary Br2-based energy storage devices are rarely advanced. Here, we introduce an electrochemical active parasite Br2 to the Ti3C2TXMXene host and construct an advanced aqueous zinc redox battery via a facile electrodeposition process (Br-Ti3C2TX). Both ex situ experimental characterizations and density functional theory (DFT) simulations have validated the natural affinity between MXenes and Br species, which is manifested as their spontaneous fixation accompanied by rapid transfer of electrons in the interface region and interlayer confinement. Consequently, the battery delivers a high-voltage plateau at 1.75 V that contributes to an improved energy density of 259 Wh kg–1Br (144 Wh kg–1Br-Ti3C2TX), exhibiting efficient output capability in the high-voltage region. Besides, benefiting from enhanced redox kinetics, the capacity achieved at −15 °C approaches to 69% of the value at room temperature. More importantly, an excellent 10 000 cycles at −15 °C with negligible capacity decay is identified. The paradigm represents a step forward for developing stationary aqueous metal-Br2 batteries.
研究领域:
材料科学
·
电化学
·
能源存储
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产品关联
DOI
PubMed
高影响因子
Scientific Reports
·
2016
·Vol. 6
·期 1
·1-13
·
IF 5.228
Cagnetta Giovanni,Liu Han,Zhang Kunlun,Huang Jun,Wang Bin,Deng Shubo,Wang Yujue,Yu Gang
Brominated organic pollutants are considered of great concern for their adverse effect on human health and the environment, so an increasing number of such compounds are being classified as persistent organic pollutants (POPs). Mechanochemical destruction is a promising technology for POPs safe disposal because it can achieve their complete carbonization by solvent-free high energy ball milling at room temperature. However, a large amount of co-milling reagent usually is necessary, so a considerable volume of residue is produced. In the present study a different approach to POPs mechanochemical destruction is proposed. Employing stoichiometric quantities of Bi 2 O 3 or La 2 O 3 as co-milling reagent, brominated POPs are selectively and completely converted into their corresponding oxybromides (i.e. BiOBr and LaOBr), which possess very peculiar properties and can be used for some actual and many more potential applications. In this way, bromine is beneficially reused in the final product, while POPs carbon skeleton is safely destroyed to amorphous carbon. Moreover, mechanochemical destruction is employed in a greener and more sustainable manner.
研究领域:
环境科学
·
化学工程
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产品关联
DOI
PubMed
高影响因子
Environmental Chemistry Letters
·
2021
·Vol. 19
·期 4
·3517-3522
·
IF 9.027
Liu Hui,Qiu Xiaojun,Li Zhi,Zhu Xiaomei,Sun Bing,Zhang Xiaoxing
Dissolved organic matter (DOM) in waters, soils, sediments, and organic waste is considered to have major role in the photochemical generation of emerging organobromine contaminants, yet mechanisms are unclear. Here we fractionated soil humic acids into bound quinone-like substances and an effluent fraction, using a new emodin-imprinted polymer. We tested the effect of these fractions on the photobromination of phenol with bromide. Results show that quinone-like substances induce three times more bromophenols than the effluent fraction. Our findings reveal a new method to separate reactive compounds from DOM and imply that formation of organobromine contaminants may be controlled by the composition of organic matter.
研究领域:
环境化学
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光化学
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分析化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Ruohan Li,Lixun Zhang,Ying Zhang,Zhengfang Zhang,Yuntao Guan
Tetrabromobisphenol A (TBBPA), currently the most widely used brominated flame retardant, has attracted significant attention. However, traditional methods for deep debromination or mineralization of TBBPA usually include multiple steps and require external oxidants. In this study, we report a complete degradation of TBBPA through a one-step process of only adding a layered double oxide-supported sulfurized nanoscale zero-valent iron (S-nZVI@LDO) under ambient conditions. TBBPA was rapidly removed by S-nZVI@LDO with an efficiency of 95.6 % (10 mg⋅L -1 ) within 12 h. The kinetic rate constant (0.0035 min −1 ) was greater when compared with traditional reductants. The produced Br - ion occupied 76.7 % of total Br content, and the concentration of total organic carbon decreased by over 50 %, suggesting a deep debromination and mineralization of TBBPA by S-nZVI@LDO. It is caused by the substantial improvement of electron transfer, O 2 adsorption, and hydrophobicity of S-nZVI@LDO facilitating synchronous reductive debromination and O 2 activation to produce · O 2 – and · OH, as approved by electrochemical test, O 2 -TPO analysis, EPR analysis, and density functional theory calculations. The enriched structural S(−II) and enhanced Fe(III)/Fe(II) redox cycling exerted vital roles in maintaining the reduction potential of the composite. The degradation pathways analysis confirmed that debromination-mineralization mechanisms dominated the complete degradation of TBBPA. This study demonstrates the feasibility of the one-step mineralization removal of TBBPA only using S-nZVI@LDO under ambient conditions and offers insight into external oxidant-free in-situ elimination of halogenated persistent organic pollutants in a natural environment.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING & TECHNOLOGY
·
2016
·Vol. 39
·期 8
·1445-1450
·
IF 2.385
Qiulin Deng,Ruwei Shen,Rong Ding,Lixiong Zhang
2,4,5-Trifluorobromobenzene is a valuable intermediate with important application in the synthesis of biologically active peptides and fluorescent reagents. A continuous-flow system has been successfully developed for the synthesis of 2,4,5-trifluorobromobenzene in a microreactor using FeBr 3 as a catalyst, which is steadily generated in situ from the reaction of Br 2 and Fe. The procedure is efficient and easy-to-handle, and 2,4,5-trifluorobromobenzene can be obtained within minutes in high yields.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL POLLUTION
·
2021
·
IF 8.071
Jing Sun,Taijun Hang,Ling Cao,Xialei Fan,Youlong Feng,Li Tan,Keyu Li,Qinyi Wang,Yingxiang Liu,Gongjun Yang
China produces and consumes large quantities of brominated flame retardants (BFRs) as well as several other unregulated electronic waste recycling activities, causing high BFR concentrations in the natural environment. Thus, Traditional Chinese Medicines (TCMs) may be contaminated by legacy BFRs (e.g. polybrominated diphenyl ethers (PBDEs)) and emerging BFRs (eBFRs, such as decabromodiphenyl ethane (DBDPE)) during growth, processing, packaging, and transportation. Pheretima , which is a typical animal drug recorded in Chinese Pharmacopoeia , was used as an example to evaluate human exposure to BFRs through TCM intake. This study is the first to determine 25 PBDEs and 5 eBFRs in Pheretima and estimate the daily BFR intake via Pheretima -containing TCMs. Twenty-seven Shanghai Pheretima and fifty-one Guang Pheretima samples were collected between March and June 2019 in southeast China. High BFR detection frequencies were found in Pheretima , of which BDE-209 and DBDPE were the most predominant analytes. The total PBDE contents ranged from 73 pg/g to 8,725 pg/g, while that of the eBFRs varied between 115 pg/g and 2,824 pg/g. The profiles and abundances were found to be species- and origin-dependent. However, the traditional processing of Pheretima may reduce BFR residues. Based on the usual clinical doses of Pheretima and the available chronic oral reference doses of BDE-47, 99, 153, and 209, the mean (95th percentile) of the total hazard quotient was estimated to be 9.1 × 10 −5 (2.7 × 10 −4 ). Therefore, there is little risk related to BFR exposure for patients taking formulated Pheretima -containing TCMs. However, it is necessary to establish routine monitoring programs for the co-existence of pollutants in TCMs to perform a systematic and comprehensive risk assessment.
研究领域:
环境科学
·
药学
·
毒理学
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2016
·
IF 3.698
Weiping Xie,Wei Dong,Deyang Kong,Yuefei Ji,Junhe Lu,Xiaoming Yin
Sulfate radicals (SO 4 − ) generated by activation of peroxymonosulfate (PMS) and persulfate (PS) are highly oxidative and applied to degrade various organic pollutants. This research was designed to investigate formation of halogenated by-products in Co 2+ activated PMS process in the presence of halides and natural organic matter (NOM). It was revealed that no halogenated by-products were detected in the presence of Cl − while 189 μg/L bromoform and 100.7 μg/L dibromoacetic acid (DBAA) were found after 120 h when 2 mg/L NOM, 0.1 mM Br − , 1.0 mM PMS, and 5 μL Co 2+ were present initially. These products are known as disinfection by-products (DBPs) since they are formed in water disinfection processes. Formation of DBPs was even more significant in the absence of Co 2+ . The data indicate that both PMS and SO 4 − can transform Br − to reactive bromine species which react with NOM to form halogenated by-products. Less DBP formation in Co 2+ -PMS systems was due to the further destruction of DBPs by SO 4 − . More DBPs species including chlorinated ones were detected in the presence of both Cl − and Br − . However, more brominated species produced than chlorinate ones generally. The total DBP yield decreased with the increase of Cl − content when total halides kept constant. This is one of the few studies that demonstrate the formation of halogenated DBPs in Co 2+ /PMS reaction systems, which should be taken into consideration in the application of SO 4 − based oxidation technologies .
研究领域:
环境科学
·
水处理技术
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jingxuan Yang,Dongxu Qu,Jue Wang,Yangtao Wu,Lingjun Bu,Yuanxi Huang,Shiqing Zhou
The N-Br bond in monobromoamine (NH 2 Br) can be cleaved by UV irradiation to generate Br • and subsequently HO • , resulting in an advanced oxidation condition (i.e., UV/NH 2 Br). This study investigated the degradation of six contaminants of emerging concern (CECs) in the UV/NH 2 Br process, including the phenolic hydrocarbons phenol and bisphenol A (BPA), the amines aniline and sulfadiazine (SDZ), and the persistent organic pollutants ibuprofen (IBP) and carbamazepine (CBZ). The results showed that UV/NH 2 Br process significantly improved the degradation of CECs following pseudo-first order kinetics, and the degradation of CECs was enhanced with the increase of NH 2 Br dosage. UV/NH 2 Br was more efficient in degrading CECs containing phenolic hydroxyl groups (100 %), followed by those containing amine groups (> 95 %). The degradation efficiency was influenced by the pH value and was highest at pH 7. It was found that low concentrations of Cl − (< 0.5 mM ) and HCO 3 − (< 0.5 mM) promoted the degradation of SDZ and IBP, but further increases in Cl − and HCO 3 − (0.5 ∼ 5.0 mM) resulted in inhibition. SDZ and IBP degradation was inhibited by photo absorption competition and free radical depletion in natural organic matter and actual water. Probe experiments showed that reactive bromine species (RBS), reactive nitrogen species (RNS), and hydroxyl radical (HO • ) played a dominant role in CEC degradation. During the degradation of IBP by UV/NH 2 Br, hydroxylation, bromination , and quinylation were proposed as the primary reaction mechanisms. As compared to HOCl disinfection, NH 2 Cl disinfection after the UV/NH 2 Br process produced lower concentrations of disinfection by-products (DBPs).
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL TOXICOLOGY
·
2021
·Vol. 36
·期 8
·1674-1682
·
IF 4.119
Jun Shi,Xueting Wang,Lulu Chen,Huiping Deng,Min Zhang
Brominated flame retardants (BFRs), such as, 1,2,5,6-tetrabromocyclooctane (HBCD), 1,2-dibromo-4-(1,2-dibromopropyl)cyclohexane (TBECH), and 1 1,2-bis-(2,4,6-tribromophenoxy)ethane (BTBPE), have garnered increasing attention due to their potent biological effects. In the present study, the toxicity of HBCD, TBECH, and BTBPE in human vascular endothelial cells (ECs) was explored. The data showed that HBCD, TBECH, and BTBPE induced cytotoxicity, namely dose–dependent cell viability reduction, cell membrane permeability and apoptosis increase, migration, and lumen formation inhibition. Moreover, HBCD was found to be more toxic than BTBPE or TBECH. Exposure to HBCD, TBECH, and BTBPE led to the production of reactive oxygen species, mitochondrial superoxide generation, and mitochondrial membrane potential collapse, implying that reactive stress caused the cytotoxicity. The ATP content, glutathione content, superoxide dismutase, and MDA activities were reduced, indicating that mitochondrial dysfunction may be the key mechanisms responsible for apoptosis. The present study suggested that mitochondria are a new target of BFRs in ECs and further deepened our understanding of the developmental toxicity of BFRs.
研究领域:
毒理学
·
细胞生物学
·
环境健康
✓ 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）