SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Menglan Gao,Zhibin Jiang,Xiaobin Liao,Xingji Bai,Huan Qi,Jing Zou,Wei Cao
Unsymmetrical dimethylhydrazine (UDMH) is found to generate substantial carcinogenic nitroso-dimethylamine (NDMA) during ozonation , moreover, its formation is promoted by ubiquitous bromide ions (Br − ) in water matrixes, but the mechanism is still unclear. In this study, effects of Br − on NDMA formation during ozonation of UDMH were studied, meanwhile, its promotion pathways were also determined. The results demonstrated that Br − promoted NDMA formation from UDMH during ozonation, the formation rate constant with Br − is over 7 times of that without Br − . NDMA amount raised from 142.5 to 327.5 μg/L when Br − dosages increased from 0 to 100 μM. No matter with or without Br − , the augment of O 3 dosages facilitated NDMA formation; the maximum value was achieved at pH 8. NDMA decreased dramatically from 173.8 to 123.5 μg/L with HCO 3 − raising from 0 to 160 μM, while increasing remarkably to 222.5 μg/L with SO 4 2− dosing. In addition, NOM inhibited NDMA formation from UDMH during ozonation. The mass spectrum of LC-MS/MS verified that the generation of Br-UDMH was main cause for promoting NDMA formation. Moreover, hypobromous acid (HBrO) was confirmed to be responsible for Br-UDMH formation. In addition, the position that oxidants and Br − attacked was demonstrated based on Gaussian calculation. The results of this study could provide theoretical basis for the application of ozonation in bromine-containing water matrixes.
研究领域:
环境科学
·
毒理学
·
化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Menglan Gao,Xiaobin Liao,Shuting Chen,Xiaoying Li,Yirou Zhang,Chao Chen,Huan Qi
Bromide ion (Br - ) in water sources has been found to affect the formation of carcinogenic non-brominated N-nitrosodimethylamine (NDMA) during ozonation of typical amines. The increasing bromide levels bring more concern due to climate change and industrial discharge, but its effects on actual water matrixes were still unclear. In this study, NDMA formation from three actual water matrixes during ozonation as the Br - concentration increased from 0 to 100 µM were investigated (promotion (100.4 ∼ 231.6 ng/L), promotion then inhibition (399.5 ∼ 461.2 ∼ 428.2 ng/L), and subtle influence (51.9 ± 6.9 ng/L)); from which the NDMA precursors were screened and 8 precursors were selected for exploring the influencing mechanisms. The results indicated that the roles of Br - on NDMA formation significantly depended on the water characteristics of actual matrixes. A total of 16 typical NDMA precursors, which were mainly derived from industrial, agricultural and pharmaceutical sources, were identified. Moreover, 6 brominated substance (Br-DMA, Br-UDMH, Br-DMSC, Br-DMS, Br-TMDS, Br 2 -TMDS), which were thought to play a crucial role in promoting NDMA formation, were also identified in actual water by precursor ion scan (PIS) method. Hypobromous acid (HOBr), which has been proved to be the culprit to the generation of brominated substances, tend to attack the electron-donating groups of amines, such as acylamino (–NHCO-R) or amidogen (–NH 2 ) groups. However, the reactive bromine species (∙Br and ∙Br 2 - ) was inclined to attack the aromatic and anti-oxidant moieties then result in Br - release, as no bromine substitution but free radical transfer reaction occurs. Therefore, decreasing HOBr formation is the crucial step to reduce NDMA generation. This work would provide technical guide for NDMA risks control during ozonation of Br - -amines co-containing water matrixes.
研究领域:
环境科学
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化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xin Liu,Qi Fu,Peng Xu,Pengfei Zhu,Zhuoyu Yang,John C. Crittenden
A sensitive spectrophotometric method (the Br − -ABTS method) for measuring monopersulfate (PMS) of 0–20 μM in water was established. The Br − -ABTS method was based on the oxidation coloration reaction where Br − as catalyst promoted PMS for oxidation of ABTS forming the green-colored ABTS radical (ABTS • + ) under pH 3.0 (50 mM phosphate buffer). ABTS • + could be quantitatively measured at 415 nm, 650 nm, 732 nm and 820 nm using UV–vis spectrophotometer. There was a well linear relationship between the absorbance of ABTS • + and PMS concentration with the value of R 2 being 0.999. The proposed Br − -ABTS method was highly sensitive, and the absorbance generated by Br − -ABTS at 415 nm was 6.59 × 10 4 cm −1 per M (mol L –1 ) of PMS. The changes of pH from 3.0 to 9.0 had an insignificant effect on the calibration curve of Br − -ABTS method. The reaction of PMS with ABTS had a stoichiometric coefficient of 1:1.96 at the pH 3.0. The residual absorbance of ABTS •+ in ultrapure water, Xiangjiang water and Hou-lake water was stable within 30 min. Moreover, the trace PMS concentration of 0.03–20 μM in ultrapure water, 0.05–20 μM in natural water (e. g. Xiangjiang water and Hou-lake water) and 1–20 μM in wastewater was accurately measured with the proposed Br − -ABTS method. Additionally, the interference of natural water matrix (e. g. humic acid), metal ions (e. g. Co(II), Fe(III) and Cu(II)) and hydroxylamine had barely interference for the proposed Br − -ABTS method. Furthermore, the Br − -ABTS method was more accurate and flexible to determine PMS concentration than DPD method during the decolorization of rhodamine B in the Co(II)/PMS system, Cu(II)/PMS system and hydroxylamine/Fe(III)/PMS process.
研究领域:
环境科学
·
分析化学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-7
·
IF 17.694
Song Yongbo,Li Yingwei,Zhou Meng,Li Hao,Xu Tingting,Zhou Chuanjun,Ke Feng,Huo Dayujia,Wan Yan,Jie Jialong,Xu Wen Wu,Zhu Manzhou,Jin Rongchao
The growth of nanoparticles along one or two directions leads to anisotropic nanoparticles, but the nucleation (i.e., the formation of small seeds of specific shape) has long been elusive. Here, we show the total structure of a seed-sized Au 56 nanoprism, in which the side Au{100} facets are surrounded by bridging thiolates, whereas the top/bottom {111} facets are capped by phosphine ligands at the corners and Br − at the center. The bromide has been proved to be the key to effectively stabilize the Au{111} to fulfill a complete face-centered-cubic core. In femtosecond electron dynamics analysis, the non-evolution of transient absorption spectra of Au 56 is similar to that of larger-sized gold nanoclusters ( n > 100), which is ascribed to the completeness of the prismatic Au 56 core and an effective electron relaxation pathway created by the stronger Au-Au bonds inside. This work provides some insights for the understanding of plasmonic nanoprism formation.
研究领域:
材料科学
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纳米技术
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物理化学
✓ 已验证
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 106
·104693-104698
·
IF 3.289
Guo Jian-feng,Hou Chang-jun,Yang Mei,Huo Dan-qun,Fa Huan-bao
In this work, we have developed a simple, cost-effective and sensitive fluorescent method for the selective determination of chromium(VI) ions (Cr(VI)) in aqueous solution. In the presence of bromide ions (Br−), the strong oxidization of Cr(VI) enables it to selectively etch the bovine serum albumin-stabled gold nanoclusters (BSA-Au NCs) and formed AuBr2− complexes. Proportional fluorescence quenching of BSA-Au NCs induced by the leaching process was closely connected with concentrations of Cr(VI) and thus provided a new detecting strategy towards Cr(VI). Under optimal conditions, the amount-dependent fluorescent response was linearly correlated with the Cr(VI) concentrations ranging from 1.0 nM to 2.5 μM over 3 orders of magnitude, with a detection limit down to 0.6 nM. The as-developed strategy also performed satisfactory selectivity as well as excellent reproducibility. Moreover, this method had been successfully applied to monitor Cr(VI) with real river water samples which demonstrated the potential for field applications.
研究领域:
分析化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Zhaochang Wu,Sijie Ge,Ying Han,Mengchen Zong,Shilong He,Jie Zhang
Heterogeneous catalytic ozonation is widely used in advanced treatment for the removal of refractory organics from bio-treated coking wastewater. However, the effect of inorganic anions on quinoline removal by catalytic ozonation remains unclear. In this study, the effect of three inorganic anions including Cl - , Br - , SO 4 2- on performance and mechanism for quinoline removal by TiO 2 catalyst was investigated. Results indicated that all three anions have inhibitory effects on quinoline removal; meanwhile Br - exhibited the strongest inhibition. Furthermore, the effect of factors including initial solution pH, ozone concentration, catalyst dosage and coexistence of anions on Br - inhibition was explored. The Br - inhibition mechanism was further systematically analyzed by characterizing the physicochemical properties of catalysts and investigating free radicals and quinoline degradation pathways. The inhibition caused by Br - became stronger with the coexistence of SO 4 2- . The presence of Br - reduced the amount of oxygen vacancies and active sites on catalysts. Also, the activity and stability of catalysts decreased because of the Ti ions leaching, which was obviously exacerbated as the coexistence of SO 4 2- . Moreover, the Br - and SO 4 2- both could react with •OH to form abundant RHS (BrOH •- , Br• and Br 2 •- ) with low oxidative activity to further inhibit quinoline removal. The radical scavenging tests demonstrated that the main reactive oxygen species (ROS) was changed from •OH to O 2 •- and 1 O 2 in the catalytic ozonation system by the introduction of Br - and SO 4 2- . Meanwhile, brominated byproducts were found to be generated during the degradation of quinoline by GC-MS analysis.
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 SCIENCE AND POLLUTION RESEARCH
·
2018
·Vol. 25
·期 18
·18001-18014
·
IF 2.8
Xu Zhengming,Han Dexia,Li Yuan,Zhang Pingling,You Lijun,Zhao Zhengang
In this study, the FPA90-Cl resin was magnetized with supported Fe 3 O 4 particles using a chemical co-precipitation method and its removal performance of bromate and coexisting precursors was explored. The magnetized FPA90-Cl resin was structurally characterized by SEM, FT-IR, and XRD. The effects of the initial concentrations, temperature, and resin dosage on bromate and bromide ion removal in drinking water were investigated using batch experiments. The magnetized FPA90-Cl resin exhibited a high removal efficiency for bromate and bromide ions at three initial concentrations, and the residual bromate concentrations were under the maximum contaminant level (MCL) of 10 μg L −1 after 80 min. The adsorption data of bromate and bromide ion could be well described by a pseudo-first-order kinetic model ( R 2 ˃ 0.98). The bromate removal alone was further studied by varying the initial solution pH, temperature, and competitive anions. The results showed that the magnetized FPA90-Cl resin could be used over a wide pH range (4.0–9.0). The maximum sorption capacity of the magnetized FPA90-Cl resin for bromate reached 132.83 mg g −1 at 298 K. The Freundlich and Redlich-Peterson isotherm models fit the bromate adsorption equilibrium better ( R 2 ˃ 0.99) than the Langmuir isotherm model ( R 2 ˃ 0.98). The thermodynamic analysis showed that the bromate adsorption process was endothermic. The negative ΔG and positive ΔS indicated that the process was spontaneous and that randomness increased after adsorption, respectively. The competition of coexisting anions with bromate was in the order of SO 4 2− > CO 3 2− > Cl − > NO 3 − > HCO 3 − > PO 4 3− . Additionally, the magnetized FPA90-Cl resin could maintain a high bromate and bromide ion adsorption capacity after five cycles of regeneration by a 0.1 M NaCl solution.
Graphical abstract
研究领域:
环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Shuyin Zhang,Jing Zou,Lingxuan Chen,Chunhua Shen,Jian Lu,Jianlin Zhang,Hangyu Cui,Geng Huang,Jun Ma
Although thermal-activated peroxymonosulfate (PMS) system possesses good performance on the removal of organic pollutants, thermal/PMS system exhibited poor capacity to remove ammonia nitrogen (NH 4 + -N). This study demonstrated the huge enhancement on the removal of NH 4 + -N by thermal/PMS system with the commonly coexistent bromide ion (Br - ). The elimination of NH 4 + -N by thermal/PMS/Br - system fitted the pseudo -zero-order kinetics model well, while the corresponding k obs in the presence of 200 μM Br - was 5.76 times greater than that by thermal/PMS system. Bromine (HBrO) was confirmed as the dominant oxidant responsible for removing NH 4 + -N and TN, while the radicals of HO ⋅ , SO 4 ⋅- and Br ⋅ were also generated but made minor contribution to removing NH 4 + -N. HBrO was mostly produced by PMS reacting directly with Br - , while these radicals were produced from the cleavage of the O-O bond in PMS and the reaction between PMS and HBrO under high temperature. Thermal/PMS/Br - system exhibited superior performance on TN removal (up to 90 %) than that by thermal/PMS system (less than 5 %) and Cl - -enhanced system (about 80 %). The main removal product of NH 4 + -N was identified as the environmentally friendly gas of N 2 , although nitrate was also detected. Neutral pH condition was the optical pH for NH 4 + -N removal. Increasing reaction temperature, PMS dosage and Br - concentration were beneficial to accelerating the removal of NH 4 + -N. Cations of Cu 2+ and Fe 3+ , anions of SO 4 2- , CO 3 2 - and NO 3 - , humic acid and the actual water matrix of landfill leachate negligibly influenced the removal of NH 4 + -N, while Cl - exhibited strong enhancement on NH 4 + -N removal. In summary, this study provided an effective method to improve the oxidizing capacity of thermal/PMS system, especially for NH 4 + -N removal in wastewater containing Br - .
研究领域:
环境科学
·
污水处理
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Xiaoyuan Song,Junjian Niu,Wenjun Yan,Xuan Li,Xiaogang Hao,Guoqing Guan,Zhongde Wang
The separation and capture of Br - ions from aqueous solutions is of great significance in view of their dual characteristics, that is, its economic value and its harmful effect on human body. In this study, BiOBr@PPy electroactive hybrid film with core-shell structure, which was fabricated by in-situ coating conductive PPy on BiOBr with ion storage space, was applied to selectively capture Br - ions using electronically switched ion exchange technology (ESIX). The capture capacity of BiOBr@PPy hybrid film reached 146.2 mg g −1 at 0.8 V oxidation voltage. While, the hybrid film had an excellent selectivity towards Br - ions in the aqueous solution with several competing anions. It was confirmed that selective Br - ion capture/release by the BiOBr@PPy hybrid film was achieved through the synergistic effect generated from sufficient Br - ions storage space of BiOBr, highly conductivity and ion screening function of PPy, and powerful driving forces jointly activated by the electrochemical redox reaction of BiOBr and PPy. In addition, the capacity retention efficiency and release rate of the hybrid film still remained above 80% after 10 cycles due to the strategy of in-situ coating of PPy. It is predicted that such a BiOBr@PPy hybrid film with synergistic effects may be a potential electroactive material for the separation and capture of Br - ions from aqueous solutions.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Shengpeng Liu,Gen Cheng,Yun Xiong,Yigang Ding,Xiaogang Luo
Due to strong activity, it is very difficult to remove low concentrations of bromide in medical wastewater by traditional method, thus highly effective and greener adsorbents should be utilized to design. In this work, the cellulose beads (CBs) were modified by the TEMPO-mediated oxidation and then bonded with Fe 3+ to fabricate Fe(III)-complexed carboxylated cellulose beads (Fe-CCBs) adsorbents. Structure and properties of Fe-CCBs were analyzed using Energy dispersive spectrum (EDS), Scanning electron microscopy (SEM), Fourier transform infrared spectrum (FT-IR), total acidity and basicity groups, X-ray diffraction (XRD), N 2 adsorption-desorption and Thermogravimetric (TGA). Moreover, batch adsorption experiments showed that the adsorption of Br − was better consistent with general-order kinetic model and Liu isotherm model, which could also further clarify the adsorption process mechanism. Meanwhile, the results revealed that removal of Br- was a spontaneous exothermic process and was more suitable to be carried out under neutral or acidic conditions. Furthermore, the mechanism of adsorption behavior of bromide ions on Fe-CCBs was based on a combination of electrostatic attraction and outer-sphere complexation. The results of this study can provide guidance for the design of novel material adsorbents and the removal of harmful anions from aqueous solutions.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
·
2024
·
IF 2.8
Lixiang Wang,Jingwen Li,Mingqiang Li,Xinping Duan,Haochen Weng,Shuailiang Xu
In this study, we introduce a novel “water-in-salt” electrolyte for Bromine-ion batteries (BIBs) for the first time: 3M AlCl 3 + 1M NH 4 Br. The 3M AlCl 3 establishes the “water-in-salt” system, while 1M NH 4 Br supplies Br- ions. Employing flexible graphite paper as the cathode, during charging, Br- cooperates with AlCl 3 , forming AlCl 3 Br - ions that embed into the graphite paper, resulting in reversible reactions during discharge. The anode utilizes various metals such as Zn, Cu, Pb, In 2 O 3 , undergoing reversible redox reactions in the charge–discharge process. The designed electrolyte effectively prevents elemental bromine generation, presenting a safe, green, and environmentally friendly aqueous electrolyte suitable for BIBs.
研究领域:
能源存储
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Shaodong Hou,Li Ling,Dionysios D. Dionysiou,Yuru Wang,Jiajia Huang,Kaiheng Guo,Xuchun Li,Jingyun Fang
Halides and natural organic matter (NOM) are inevitable in aquatic environment and influence the degradation of contaminants in sulfate radical (SO4•–)-based advanced oxidation processes. This study investigated the formation of chlorate in the coexposure of SO4•–, chloride (Cl–), bromide (Br–) and/or NOM in UV/persulfate (UV/PDS) and cobalt(II)/peroxymonosulfate (Co/PMS) systems. The formation of chlorate increased with increasing Cl– concentration in the UV/PDS system, however, in the Co/PMS system, it initially increased and then decreased. The chlorate formation involved the formation of hypochlorous acid/hypochlorite (HOCl/OCl–) as an intermediate in both systems. The formation was primarily attributable to SO4•– in the UV/PDS system, whereas Co(III) played a significant role in the oxidation of Cl– to HOCl/OCl– and SO4•– was important for the oxidation of HOCl/OCl– to chlorate in the Co/PMS system. The pseudo-first-order rate constants (k′) of the transformation from Cl– to HOCl/OCl– were 3.32 × 10–6 s–1 and 9.23 × 10–3 s–1 in UV/PDS and Co/PMS, respectively. Meanwhile, k′ of HOCl/OCl– to chlorate in UV/PDS and Co/PMS were 2.43 × 10–3 s–1 and 2.70 × 10–4 s–1, respectively. Br– completely inhibited the chlorate formation in UV/PDS, but inhibited it by 45.2% in Co/PMS. The k′ of SO4•– reacting with Br– to form hypobromous acid/hypobromite (HOBr/OBr–) was calculated to be 378 times higher than that of Cl– to HOCl/OCl–, but the k′ of Co(III) reacting with Br– to form HOBr/OBr– was comparable to that of Cl– to HOCl/OCl–. NOM also significantly inhibited the chlorate formation, due to the consumption of SO4•– and reactive chlorine species (RCS, such as Cl·, ClO· and HOCl/OCl–). This study demonstrated the formation of chlorate in SO4•–-based AOPs, which should to be considered in their application in water treatment.
研究领域:
环境科学
·
水处理工程
✓ 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）