JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Zhihao Yan,Hanyang Qian,Juanjuan Yao,Meng Guo,Xiong Zhao,Naiyun Gao,Zhi Zhang
Microplastics (MPs) in drinking water are predominantly < 10 µm. The leaching of MPs derived dissolved organic matters (MP-DOM) from 5 µm polypropylene MPs (PP-MPs) and polystyrene MPs (PS-MPs) and the formation of MP-DOM derived disinfection byproducts during chlorination disinfection were first investigated. Comparably, PS-MPs are more vulnerable to chlorination and the primary attacks are on para C in aromatic side-chains via electrophilic Cl-substitution and oxidation by two-electron transfer. The O/C and Cl/C ratio of polystyrene MPs was linear and exponential versus initial available Cl 2 concentrations, respectively. The significant PS-DOM leaching was observed with initial available Cl 2 of 4.0 mg/L (USEPA recommended upper dose). As the initial available Cl 2 concentration increased to 8.0 mg/L, the adsorption of chloro-phenolic-components of 200 Daltons in PS-DOM by 5 µm PS-MPs was observed for the first time. Trichloromethane (TCM) was identified as the dominant disinfection byproduct with a formation potential of 60.3 ± 7.8 and 73.7 ± 9.8 μg/mg for PS-DOM and PP-DOM, respectively. The derived TCM could adsorb onto PS-MPs followed the pseudo-second-order kinetic and Langmuir isotherm models. Extreme chlorination could reduce the maximal adsorption capacity of TCM on 5 µm PS-MPs from 196.68 ± 48.66 to 146.02 ± 32.98 μg/g. Thus, PS-MPs act as precursors and carriers of TCM in chlorination.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Xiang-mei Zhong,Xiang Fu,Yu-qiong Gao,Yang-yang Liu,Xue-ting Ren,Ji-yue Li,Lei Li,Nai-yun Gao
This study comparatively investigated the degradation kinetics and mechanisms, changes in toxicity, and formation of disinfection byproducts (DBPs) for two pharmaceutical contaminants (PCs), emtricitabine (FTC) and trimethoprim (TMP), using the medium-pressure UV/nitrate (MPUV/NO 3 − ) process. Alkaline conditions markedly enhanced direct MPUV photolysis of both FTC and TMP, with FTC being more susceptible than TMP. The presence of 2 mM NO 3 − enhanced degradation rate (k obs ) by 1.2–2.3-fold for FTC and 1.8–10.8-fold for TMP under MPUV across different pH conditions, attributed to •OH and reactive nitrogen species (RNS) generation. Under the MPUV/NO 3 − process, both FTC and TMP showed a decrease in k obs with increasing pH. Their k obs initially increased with NO 3 − concentration but plateaued at higher levels. Structural differences led to distinct reactive species dominating FTC and TMP degradation. Anions and humic acid inhibited FTC and TMP degradation to varying degrees. Based on LC/TOF/MS analysis and DFT calculations, the cytosine moiety in FTC and the pyrimidine ring in TMP were identified as vulnerable sites, leading to the proposed degradation pathways. Most FTC transformation products showed increased developmental toxicity but decreased mutagenicity. Nitrated TMP products exhibited notably higher developmental toxicity. The Vibrio fischeri inhibition assay showed that the MPUV/NO 3 − process had the ability to control toxicity. Pretreatment with MPUV/NO 3 − enhanced the formation of trichloronitromethane during post-chlorination. Additionally, chloramination outperforms chlorination in controlling DBPs formation and their associated toxicity. Overall, this study provides critical insights into the transformation pathways and ecological risk assessment of PCs in nitrate-rich wastewater under polychromatic UV irradiation.
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Huiming Xiang,Yisheng Shao,Naiyun Gao,Xian Lu,Wenhai Chu,Na An,Chaoqun Tan,Xuhui Zheng,Yuqiong Gao
The degradation of sulfonamides (SAs) in the presence of bromide during the UV/free chlorine process was investigated in this study. The reactions followed pseudo first-order kinetics. With increasing bromide concentrations of 1, 5, 10–20 µM, the degradation rate was gradually raised. The contribution of different reactive species has been calculated. The degradation products and DBPs formed by SAs were determined. The mechanisms of the degradation of SAs in the presence of bromide included hydroxylation, cleavage of the pyrimidinyl group, and bromine and chlorine electrophilic addition. The concentration of brominated disinfection by-products, including DBCM, TBM and DBAN, increased with increasing bromide dosage and degradation time, while 1, 1, 1-TCP and 1, 1-DCP decreased. In an acute toxicity test, the inhibition rate decreased in the first 5–10 min then increased after 10 min degradation when 10 µM Br − was added to the system. The initial decrease may due to the formation of low toxicity substances after the cleavage of the pyrimidinyl group, while the subsequent increase may be attributable to the increased formation of DBPs.
研究领域:
环境科学
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化学
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毒理学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Shengnan Chen,Jing Deng,Cheng Ye,Chengcheng Xu,Lingyi Huai,Xiao Ling,Jun Li,Xueyan Li
Pre-magnetized Fe 0 /persulfate (pre-Fe 0 /PS) process was innovatively employed for controlling the pollution of p -arsanilic acid ( p -ASA). This process showed favorable removal performance, achieving almost complete elimination of 10 mg/L p -ASA within 30 min at the reaction conditions of 0.2 g/L pre-Fe 0 and 1 mM PS. The increase of PS concentration and pre-Fe 0 dosage was conducive to the degradation. The coexistence of Cl − , NO 3 − and SO 4 2− accelerated the removal, however the presence of HCO 3 − and HA presented the opposite trend. The p -ASA degradation decelerated gradually with increasing pH from 5 to 9. Its removal was caused by the attack of reactive oxygen species (i.e., SO 4 − , OH, O 2 − ), which could be continuously formed via the Fe 2+ /Fe 3+ cycle in solution and on pre-Fe 0 surface. In pre-Fe 0 /PS system, SO 4 − in solution, surface-bound SO 4 − , OH, OH in solution, O 2 − in solution and Fe(IV) contributed to the p -ASA degradation. A plausible transformation route related to the break of C-N and As-C bonds, the substitution of OH group was put forward. More importantly, the released inorganic arsenic during p -ASA decomposition could be effectively controlled through multiple functions including the precipitation, co-precipitation and sorption, which was well confirmed by XPS, FTIR and XRD analysis. Pre-Fe 0 /PS and Fe 0 /PS pretreatments both reduced the generation of C-DBPs except for chloral hydrate, while increased the formation of N-DBPs except for trichloroacetamide.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Bao-Jun Xu,Yao Lu,Nan Liu,Ying Chen,Min Liu,Qian-Yuan Wu,Ye Du
Periodate (PI) shows promising potential as an oxidant for wastewater treatment; however, its impact on the toxicity of wastewater remains unknown. Here, we found that with 100 μM PI addition, the cytotoxicity of wastewater increased from 4.8 to 7.6 mg-Phenol/L to 9.5 to 12.8 mg-Phenol/L, and genotoxicity increased from 0.3 to 0.9 μg-4-NQO/L. Interestingly, hypoiodous acid (HOI) was not detected during the reaction, and there was no observed increase in the concentration of total organic iodine (TOI). CHON components in dissolved organic matter changed most obviously in PI oxidation, which might serve as primary precursors for toxic byproducts. Cytotoxicity of typical nitrogen-containing precursors of tryptophan, lysine, phenylalanine, and tyrosine after PI oxidation increased from not detected to 14.7, 2.4, 4.1, and 3.2 mg-Phenol/L, respectively. Here, four nonhalogenated aromatic nitrogenous byproducts (N-DBPs) of 3-hydroxyquinoline, 4-hydroxyquinoline, benzopyridine, and benzopyrrole were confirmed using standards, and four byproducts such as 2-formylbenzonitrile were tentatively proposed. The cytotoxicity of the four confirmed byproducts was comparable to those known N-DBPs such as nitrosamines, suggesting attention should be given to these nonhalogenated but nitrogenous byproducts. The four confirmed byproducts were detected in two PI-treated wastewater samples with concentrations of 0.8, 0.98, 0.52, and 0.0038, and 18.28, 1.50, 0.57, and 0.0074 μg/L, respectively, with contributions less than 1.5% to the overall cytotoxicity. Further investigations are warranted to elucidate the primary drivers of toxicity in PI-treated wastewater.
研究领域:
环境科学
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水处理
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毒理学
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化学工程
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2024
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IF 10.8
Shaoyang Hu,Xiangxiang Li,Guangzhao Li,Zhigang Li,Falin He,Guang Tian,Xingchen Zhao,Rutao Liu
Recently, seven dihalohydroxybenzonitriles (diHHBNs) have been determined as concerning nitrogenous aromatic disinfection byproducts (DBPs) in drinking water. Herein, eight new monohalohydroxybenzonitriles (monoHHBNs), including 3-chloro-2-hydroxybenzonitrile, 5-chloro-2-hydroxybenzonitrile, 3-chloro-4-hydroxybenzonitrile, 3-bromo-2-hydroxybenzonitrile, 5-bromo-2-hydroxybenzonitrile, 3-bromo-4-hydroxybenzonitrile, 5-iodo-2-hydroxybenzonitrile, and 3-iodo-4-hydroxybenzonitrile, were detected and identified in drinking water for the first time. Thereafter, the relative concentration–cytotoxicity contribution of each HHBN was calculated based on the acquired occurrence level and cytotoxicity data in this study, the genome-scale cytotoxicity mechanism was explored, and a quantitative structure–activity relationship (QSAR) model was developed. Results indicated that new monoHHBNs were present in drinking water at concentrations of 0.04–1.83 ng/L and exhibited higher cytotoxicity than some other monohalogenated aromatic DBPs. Notably, monoHHBNs showed concentration–cytotoxicity contribution comparable to diHHBNs, which have been previously identified as potential toxicity drivers in drinking water. Transcriptomic analysis revealed immunotoxicity and genotoxicity as dominant cytotoxicity mechanisms for HHBNs in Chinese hamster ovary (CHO-K1) cells, with potential carcinogenic effects. The QSAR model suggested oxidative stress and cellular uptake efficiency as important factors for their cytotoxicity, highlighting the importance of potential iodinated HHBNs in drinking water, such as 3,5-diiodo-2-hydroxybenzonitrile, for future studies. These findings are meaningful for better understanding the health risk and toxicological significance of HHBNs in drinking water.
研究领域:
环境化学
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毒理学
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基因组学
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水处理
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2021
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IF 7.086
Guilin He,Tuqiao Zhang,Qingzhou Zhang,Feilong Dong,Yonglei Wang
Enoxacin (ENO) is widespread in water because it is commonly used as a human and veterinary antibiotic. However, little effort has been dedicated to revealing the transformation mechanisms of ENO destruction using ClO 2 , especially within a water distribution system (WDS). To address this knowledge gap, the kinetics, byproducts, toxicity, and formation potential of halogenated disinfection byproducts (DBPs) associated with ENO destruction using ClO 2 in a pilot-scale PE pipe was explored for the first time. Statistical analyses showed that the destruction efficiency of ENO in the pilot-scale PE pipe was lower than that in deionized water (DI water), and the reactions in DI water followed the second-order kinetic model. Furthermore, pH has a significant effect on the destruction of ENO, and the removal ratio increased at a higher pH. Additionally, increasing the flow rate elevated the ENO removal efficiency; however, the influence of flow velocity was limited to ENO destruction. The ENO removal rates within the diverse pipes exhibited the following order: stainless steel pipe < PE pipe < ductile iron pipe. Nine possible intermediates were identified, and those that were formed by piperazine group cleavage represented the major primary byproducts of the entire destruction process. Additionally, the ENO destruction in a pilot-scale PE pipe had minimal influence on halogenated DBPs and chlorite formation. Finally, the toxicity evaluation illustrated that the presence of ENO increased the potential risk of water quality safety when treated with ClO 2 .
研究领域:
环境科学
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公共卫生
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化学工程
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2023
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IF 9.8
Weiwei Bi,Xin Zhang,Lei Wang,Yuzhe Ding,Shijun Zhu,Xiaoyan Ma,Qingsong Li,Xueyan Li,Jing Deng
This study systematically compared the degradation kinetics, conversion pathways, formation of disinfection by-products (DBPs), and changes in toxicity for sulfamethazine and carbamazepine in UV/nitrate system. Additionally, the study simulated the generation of DBPs in the post-chlorination process after the introduction of bromine ions (Br − ). The contributions of UV irradiation, hydroxyl radicals ( • OH), and reactive nitrogen species (RNS) to SMT degradation were determined to be 28.70 %, 11.70 %, and 59.60 %, respectively. The contributions of UV irradiation, • OH, and RNS to CBZ degradation were found to be 0.00 %, 96.90 %, and 3.10 %, respectively. A higher dosage of NO 3 − facilitated the degradation of both SMT and CBZ. Solution pH posed almost no effect on SMT degradation, while acidic conditions favored CBZ removal. The degradation of SMT was found to be slightly promoted at low concentrations of Cl − , while the presence of HCO 3 − significantly accelerated the degradation. Cl − , as well as HCO 3 − , retarded the CBZ degradation. Natural organic matter (NOM) as a free radical scavenger and UV irradiation filter posed a substantial inhibitory effect on the degradation of SMT and CBZ. The degradation intermediates and transformation pathways of SMT and CBZ by UV/NO 3 − system were further elucidated. The results showed that the main reaction pathways were bond-breaking reaction, hydroxylation, and nitration/nitrosation reaction. The acute toxicity of most of the intermediates generated during SMT and CBZ degradation was reduced after UV/NO 3 − treatment. After treatment of SMT and CBZ in UV/nitrate system, the DBPs generated in subsequent chlorination were mainly trichloromethane and a small amount of nitrogen-containing DBPs. After bromine ions were introduced in UV/NO 3 − system, a large amount of the originally generated trichloromethane was converted to tribromomethane.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
CHEMOSPHERE
·
2025
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IF 8.1
Danming Wen,Junyao Wang,Miaomiao Ding,Aikeyidanmu Zhamaerding,Xialin Hu,Daqiang Yin
Iodinated disinfection by-products (I-DBPs) have raised concerns due to their potential cytotoxicity and genotoxicity compared to chlorine and bromine-based by-products. In aquaculture, high-dose iodine-based disinfectants can react with natural organic matter (NOM) in water, generating significant amounts of I-DBPs that might pose environmental risks. This research explored the reaction characteristics of I-DBPs by using two commonly used iodine-based disinfectants (iodine tincture and Polyvinylpyrrolidone-iodine (PVP–I)) in aquaculture. The results indicated that controlling pH at around 8.0 effectively reduced I-DBP formation. A higher concentration of PVP-I (10 μM) was required to produce triiodomethane (TIM) compared to iodine tincture (2.5 μM), likely due to the slower release of iodine from PVP-I. The concentrations of I-DBPs showed a multiplicative growth trend as the concentrations of the iodine-based disinfectants increased. Humic acid (HA) demonstrated a stronger potential for I-DBP formation than algal-derived organic matter (AOM), including extracellular organic matter (EOM) and intracellular organic matter (IOM), due to its strong electron-withdrawing aromatic structure. While EOM led to a greater variety of I-DBPs, IOM contributed more significantly to TIM formation at higher disinfectant concentrations, probably due to its large molecular size and abundance of reactive carbon atoms. The I-DBP formation patterns in the aquaculture water are similar to those of HA, possibly due to the presence of similar compositional components, such as lignin and proteins. The study provides important insights for optimizing iodine disinfectant use in aquaculture and managing I-DBP risks.
研究领域:
环境科学
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水产养殖
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水化学
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毒理学
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消毒副产物
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Haoran Yin,Qizhan Zhang,Yi Su,Yunping Tang,Minghua Zhou
To promote the performance of traditional UV/chlorine and UV/H 2 O 2 processes, the novel UV based advanced oxidation process with electrochemical co-generation of chlorine and H 2 O 2 (UV/E-Cl&H 2 O 2 ) was for the first time used for degradation of carbamazepine (CBZ), a refractory antiepileptic drug with resistance to photodegradation and microbial degradation . Compared with UV/E-Cl and UV/E-H 2 O 2 processes, the apparent first-order rate constant of CBZ degradation by UV/E-Cl&H 2 O 2 process increased by 3.87 and 5.84 times respectively with a lower energy consumption (1.12 kWh/m 3 -log). Meanwhile, the disinfection by-products (DBPs) formation by the novel process was 21.4% less than that by UV/E-Cl process. Under the optimal condition of initial pH 7, applied current 600 mA and 15 mM NaCl, the UV/E-Cl&H 2 O 2 process could almost completely eliminate CBZ within 4 min and obtain 57.8% TOC removal in 1 h. The mechanism of UV/E-Cl&H 2 O 2 was investigated through processes comparison, quenching experiments, EPR analysis and determination of OH concentration. The generated radicals (i.e., OH and reactive chlorine species), especially OH, played a major role in CBZ removal. Besides, the possible degradation pathways of CBZ were proposed and the stability of UV/E-Cl&H 2 O 2 process for CBZ removal was certified based on ten consecutive runs. The degradation of typical pollutants (sulfamethazine, rhodamine B, methylene blue , atrazine and phenol) and treatments in three kinds of real wastewater confirmed the wide application feasibility of the novel process. In summary, this study provides a novel efficient and energy-saving process for removing organic pollutants with promising perspectives..
研究领域:
环境科学
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水处理
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化学工程
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高级氧化过程
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2020
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IF 6.551
Guiqiao Wang,Weiye Shi,Defang Ma,Baoyu Gao
Bisulfite-activated permanganate (PM/BS) oxidation process can oxidize ciprofloxacin in complex water matrices rapidly. However, effects of PM/BS pre-oxidation on the formation of disinfection byproducts (DBPs) during post-chlorination of ciprofloxacin-contaminated waters need to be addressed. This study investigated the formation of trihalomethanes (THMs), haloacetonitriles (HANs), haloketones and trichloronitromethane during chlorination of ciprofloxacin-contaminated humic acid (HA), bovine serum albumin (BSA) and alginate solutions, and revealed the effects of PM/BS pre-oxidation on ciprofloxacin degradation and DBP formation during post-chlorination, considering the presence of Br − . Only THMs and HANs were quantifiable. THMs were the most abundant. Ciprofloxacin-contaminated HA exhibited the highest formation potential of DBPs and integrated toxic risk value (ITRV). In the absence of Br − , PM/BS pre-oxidation reduced or hardly affected the toxicity risks derived from DBPs formed from the post-chlorination. However, the presence of Br − greatly reduced the degradation of ciprofloxacin (30–50%) in various waters. In the ciprofloxacin-contaminated waters containing Br − , the total ITRVs of DBPs formed from post-chlorination increased by 60%–800% with PM/BS pre-oxidation, attributing to the enhanced formation of DBPs especially bromochloroacetonitrile and dibromoacetonitrile. Overall, PM/BS is a potential pre-oxidation technology for the treatment of ciprofloxacin-contaminated waters without bromide.
研究领域:
环境科学
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水处理
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化学工程
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毒理学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lei Wang,Hong Wang,Sinong Huang,Jiao Feng,Yifei Wu,Jing Deng,Junping Liu,Xiang Tu,Xiaoyan Ma,Xueyan Li,Andrea M. Dietrich
Complete dehalogenation of halogenated organic pollutants has attracted increasing attention, and electrocatalytic reduction processes are considered prospective technologies due to their high selectivity for carbon-halogen bonds. In this study, a vitamin B 12 (VB 12 ) composite electrode was prepared and applied to remove the refractory tribromoacetic acid (TBAA). The reduction process dominated by the VB 12 composite electrode showed a degradation efficiency of 55.2 % for 200 μg/L TBAA within 60 min. Interestingly, UV irradiation considerably increased the efficiency of TBAA for dehalogenation on the VB 12 composite electrode. The photoelectrochemical co-catalytic system of a VB 12 composite electrode coupled with UV (LP UV 254 nm) could remove 92.2 % of TBAA in 20 min with a rate constant 12 times higher than the VB 12 -only electrolysis system. The in situ Raman characterization and cyclic voltammetry tests confirmed that the accelerated formation of Co-Br bonds and the enhanced atomic H* mediated ability were responsible for improving debromination efficiency. The degradation of TBAA mainly underwent chemical reactions of debromination and mineralization. Acetic acid, formic acid, formaldehyde, and Br - were the major transformation products of TBAA. Acidic conditions favoured TBAA removal in the UV synergistic VB 12 electrolytic system, and excellent cycling stability of debromination was obtained in complex aqueous environments (actual bodies of water containing various inorganic and organic matter). This research provides an efficient dehalogenation technology for halogenated micropollutants and novel perspectives on the scientific design of photoelectrochemical dehalogenation processes.
研究领域:
环境科学
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电化学工程
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污染控制技术
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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）