SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
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IF 9.8
Tianze Liu,Xiaobin Liao,Xinna Lin,Jing Yu,Huan Qi,Zhibin Jiang,Jing Zou,Qingsong Li
This study was to evaluate the feasibility of controlling carcinogenic nitrosodiethylamine (NDEA) formation from greenhouse gas adsorbent 3-diethylaminopropylamine (DEAPA) by pre-O 3 in subsequent chlorination/chloramination processes. The result indicated that the NDEA yields (0.4 %) during chlorination was 1.3 times of that during chloramination (0.3 %); pre-oxidation with 4 mg/L O 3 significantly cut down its formation; the reduction rates were up to 67.5 and 48.5 %, respectively. OH scavenger greatly augmented the final NDEA amount from 1.86 to 5.05 μg/L during ozonation , while its roles on subsequent processes differed with disinfection methods as well as O 3 (g) dosages. Most of co-existed substances inhibited NDEA generation, except NO 2 − , CO 3 2− and SO 4 2− , which slightly promoted during ozonation. Basing on Gaussian calculation, GC/MS and UPLC-Q-TOF-MS analysis, the influencing mechanisms of pre-O 3 on NDEA formation in subsequent disinfection processes were proposed. In addition, the calculated toxicity analysis as well as the whole toxicity was applied to evaluate the possibility of pre-O 3 on risk control.
研究领域:
环境科学
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水处理工程
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毒理学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 21
·12907-12914
·
IF 3.361
Keke Ma,Lu Zhou,Yu Bai,Yiying Xin,Mingru Chen,Heping Li,Chengyu Bao,Yuexi Zhou
Gas–liquid discharge non-thermal plasma (NTP) coupled with an ozonation reactor was used to investigate the removal of a broad-spectrum antibacterial agent, chloroxylenol (PCMX), from aqueous solution. Under the same experimental conditions (discharge power of 50.25 W, the initial concentration of PCMX of 60 mg L−1, oxygen flow of 1.0 L min−1 and PCMX solution flow of 150 mL min−1), the PCMX degradation rates in the ozonation-only, NTP-only and NTP/O3 systems were 29.25%, 67.04% and 79.43%, respectively. Correspondingly, the energy efficiency has also been greatly improved, and increased to 0.45, 1.03 and 1.21 g kW−1 h−1. In addition, the effects of the initial concentration of PCMX, initial pH, the flow rate of oxygen, the addition of H2O2 and the addition of a radical scavenger on the degradation rate of PCMX were investigated in the NTP/O3 system. The degradation rate in acidic solutions was higher than that in alkaline solutions. During the removal process of PCMX, the rate of degradation was strongly increased with the addition of H2O2 and acutely decreased with the addition of the radical scavenger. Compared with deionized water the degradation rates of PCMX in secondary effluent were inhibited. Four main intermediates of PCMX degradation by the NTP/O3 system were identified by gas chromatography-mass spectrometry (GC-MS) and a possible degradation pathway of PCMX was proposed. The changes in toxicity of the PCMX solution during the NTP/O3 system oxidation process were also evaluated using bioluminescent bacteria and Quantitative Structure Activity Relationship (QSAR) models with the help of the ECOSAR software.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
·
2022
·
IF 9.988
Zhibo Zhang,Yanping Duan,Chaomeng Dai,Si Li,Yuru Chen,Yaojen Tu,Kah Hon Leong,Lang Zhou
Peracetic acid (PAA) as an emerging oxidative has been concerned increasingly due to its high oxidation capacity and low byproducts formation potential. This study was to investigate the oxidation of sulfamethazine (SMZ) by PAA activated with activated biochar (ABC) after thermal modification. The results demonstrated that PAA could be effectively activated by ABC to degrade SMZ in a wide pH range (3–9), which followed the pseudo-second-order kinetics ( R 2 > 0.99). Both non-radicals (singlet oxygen) and free radicals (alkoxy radicals, hydroxyl radicals) existed in the ABC/PAA system, and the degradation of SMZ was dominated by singlet oxygen. Humic acid (HA), SO 4 2− and HCO 3 − slightly inhibited the degradation of SMZ in the ABC/PAA process, while Cl − and Br − promoted the degradation of SMZ. The cleavage of S–N, S–C bond, and SO 2 extraction reaction rearrangement was the main oxidation process of SMZ. Meanwhile, the results of the ECOSAR program showed that the acute toxicity of most by-products was significantly reduced compared to SMZ, which revealed the potential applicability of the ABC/PAA process in the treatment of antibiotics pollution and their detoxification.
研究领域:
环境科学
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化学工程
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毒理学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jianchao Liu,Yihao Qin,Guanghua Lu,Runren Jiang
Photocatalysts are one of the effective methods to degrade antibiotic contamination, but the efficiency is low and the toxicity is not well recognized. Deep lattice doping to induce defect generation is an effective way to improve the performance of photocatalysts. Here, defect-rich bromine-doped BiOCl-XBr photocatalysts were constructed with the help of small molecules inserted into the interlayer. The photocatalytic degradation performance of BiOCl-XBr was significantly enhanced, and its degradation rate was up to about 12 times that of BiOCl monomer. The main reasons for the stronger photocatalytic performance of BiOCl-XBr include Br doping to enhance visible light absorption, surface defects, and Bi valence changes to improve charge transport. The degradation of tetracycline (TC) produced more toxic intermediates, and the biotoxicity experiments also confirmed that the toxicity showed a trend of increasing and then decreasing, indicating that the more toxic intermediates were also mineralized during the degradation process. However, the mortality and hatching rate of zebrafish in the exposed group after degradation recovered but changed their activity pattern under light and dark conditions. This further warns us to focus on the toxicity changes after antibiotic degradation. Finally, based on the free radical analysis, the mechanism of photocatalytic degradation and detoxification of TC by BiOCl-XBr was proposed.
研究领域:
环境科学
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材料科学
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生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Wen-Long Wang,Qian-Yuan Wu,Zhi-Ming Li,Yun Lu,Ye Du,Ting Wang,Nan Huang,Hong-Ying Hu
Carbamazepine (CBZ) is a ubiquitous micropollutant in wastewater and reclaimed water. In this study, we evaluated CBZ degradation by light-emitting diode (LED)-driven UV/chlorine oxidation. Under LED irradiation of 280 nm (LED280) and 310 nm (LED310), UV/chlorine could efficiently degrade CBZ. Compared with LED UV/H 2 O 2 treatment, LED UV/chlorine oxidation achieved a CBZ degradation rate that was one order of magnitude higher. The CBZ degradation followed pseudo-first-order kinetics, and the rate constants ( k obs,CBZ ) for LED280 UV/chlorine and LED310 UV/chlorine increased from 0.072 to 0.91 min −1 and 0.044 to 0.65 min −1 , respectively, when chlorine dosage increased from 0.07 to 0.14 mM. Under neutral conditions, the generated OH and Cl accounted for over 80% of the CBZ degraded by LED UV/chlorine. The maximum k obs,CBZ for LED UV/chlorine was observed at pH 8.5; k obs,CBZ decreased when solution pH increased to 9.5 or decreased to 5.5. This is because the main UV-absorbing chlorine species in the LED280 and LED310 systems is OCl − , which is different from those in low-pressure mercury lamp/chlorine systems. The acute toxicity for CBZ solution treated by LED UV/chlorine increased at lower fluence (<752 mJ/cm 2 ) and decreased at higher fluence (>1233 mJ/cm 2 ). However, the cytotoxicity to Chinese hamster ovary cells and adsorbable organic halide content of CBZ solution both increased after chlorination and LED UV/chlorine. The lowest electrical cost for the degradation of CBZ by LED UV/chlorine occurred under neutral conditions with a chlorine dosage of 0.4–0.7 mM (28.4–49.7 mg/L).
研究领域:
环境科学
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水处理技术
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毒理学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Runren Jiang,Guanghua Lu,Tianjian Dang,Min Wang,Jianchao Liu,Zhenhua Yan
Photocatalysis is a promising method for water pollution treatment, but it is challenged due to its low efficiency and insufficient understanding of the toxicity after degradation. In this work, we construct a polyethyleneimine-enhanced BiOBr semiconductor organic framework (PEI/BiOBr SOF) by utilizing PEI's bonding and intercalation effects. PEI/BiOBr SOF enhances the photocatalytic degradation of bisphenol AF (BPAF) at a reaction rate 10 times that of BiOBr. Under the dual effects of intercalation and bonding, PEI/BiOBr SOF can realize extended the light absorption, increase the specific surface area and surface-active sites, inhibit carrier complexation, and promote the production of reactive oxygen species. The toxicity changes of the BPAF were evaluated by combining chemical product analysis and biological toxicity experiments. The mutual validation of the toxicity prediction results of the ECOASR product and the zebrafish toxicity experiment confirmed that the toxicity of BPAF decreased after degradation. Furthermore, the mechanism of photocatalytic degradation and detoxification of BPAF with PEI as the circuit of charge transmission of the BiOBr SOF was proposed.
研究领域:
环境科学
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材料科学
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毒理学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Hang Liu,Yuan Meng,Jie Li,Xiaohui Wang,Tingting Zhang
The pseudo-persistence of pharmaceutical and personal care products (PPCPs)in the aqueous environment may pose potential risks to human health and ecosystems. The UV disinfection in wastewater treatment plants is one of the essential processes before PPCPs enter the water environment, so it is crucial to elucidate the photolytic behavior and mechanism of PPCPs under UV radiation . In this work, carbamazepine (CBZ) and caffeine (CAF) were selected as typical pollutants to investigate the effect of water matrixes, humic acid , inorganic ions , and pH on the UV radiation performance. Hydroxyl radical (•OH) and singlet oxygen ( 1 O 2 ) were identified by quenching experiments and electron paramagnetic resonance (EPR) spectra as playing a dominant role in the degradation process. UPLC-TOF/MS was conducted to identify 13 and 14 possible intermediates of CBZ and CAF, respectively. Moreover, combining density functional theory (DFT) calculations (Frontier Molecular Orbital and Fukui index), hydroxylation , oxidation , and ring cleavage were proposed as the main degradation pathways of the contaminants, which occurred first at the C(7C), N(17 N) and O(18O) sites of CBZ and at the C(9C) site of CAF. The bio-acute toxicity experiment and the Ecological Structure-Activity Relationships (ECOSAR) program were performed to analyze and predict the toxicity of the intermediates of CBZ and CAF under UV radiation, respectively. The results showed that the acute toxicity of both solutions increased after UV radiation and followed with the combined toxicity. This work has great scientific value and practical environmental significance for evaluating the UV disinfection process and managing PPCPs in the aqueous environment.
研究领域:
环境科学
·
毒理学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Yandong Yang,Xiangkun Jiang,Yi Yang,Jia Wang,Yahui Zhao,Shanshan Lin,Jiao Qu,Christopher J. Martyniuk,Yuanhui Zhao,Chao Li
Liquid crystal monomers (LCMs) are a new class of emerging pollutants with high octanol-water partition coefficients; however, their transformation behavior and associated risk to environments with high organic matter content has rarely been reported. In this study, we investigated the photodegradation kinetics, mechanism, and toxicity variation of 23 LCMs on leaf wax models (e.g., organic solvents methanol and n-hexane). The order of the photolysis rates of these LCMs were biphenylethyne LCMs > phenylbenzoate LCMs > diphenyl/terphenyl LCMs under simulated sunlight, while the phenylcyclohexane LCMs were resistant to photodegradation. The phenylbenzoate and biphenylethyne LCMs mainly undergo direct photolysis, while the diphenyl/terphenyl LCMs mainly undergo self-sensitized photolysis. The main photolysis pathways are the cleavage of ester bonds for phenylbenzoate LCMs, the addition, oxidation and cleavage of alkynyl groups for biphenylethyne LCMs, and the cleavage/oxidation of chains attached to phenyls and the benzene ring opening for diphenyl/terphenyls LCMs. Most photolysis products remained toxic to aquatic organisms to some degree. Additionally, two quantitative structure-activity relationship models for predicting k obs of LCMs in methanol and n-hexane were developed, and employed to predict k obs of 93 LCMs to fill the k obs data gap in systems mimicking leaf surfaces. These results can be helpful for evaluating the fate and risk of LCMs in environments with high content of organic phase.
研究领域:
环境科学
·
毒理学
·
化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Wenyan Yu,Shaoyu Tang,Jonathan W.C. Wong,Zhujun Luo,Zongrui Li,Phong K. Thai,Minghan Zhu,Hua Yin,Junfeng Niu
N-(1,3-dimethylbutyl)-N′-phenyl-p-phenylenediamine quinone (6PPD-Q) has been identified to induce acute toxicity to multifarious aquatic organisms at exceptionally low concentrations. The ubiquity and harmful effects of 6PPD-Q emphasize the critical need for its degradation from water ecosystems. Herein, we explored the transformation of 6PPD-Q by an ultraviolet-activated peroxymonosulfate (UV/PMS) system, focusing on mechanism, products and toxicity variation. Results showed that complete degradation of 6PPD-Q was achieved when the initial ratio of PMS and 6PPD-Q was 60:1. The quenching experiments and EPR tests indicated that SO 4 •− and •OH radicals were primarily responsible for 6PPD-Q removal. Twenty-one degradation products were determined through high-resolution orbitrap mass spectrometry, and it was postulated that hydroxylation, oxidative cleavage, quinone decomposition, ring oxidation, as well as rearrangement and deamination were the major transformation pathways of 6PPD-Q. Toxicity prediction revealed that all identified products exhibited lower acute and chronic toxicities to fish, daphnid and green algae compared to 6PPD-Q. Exposure experiments also uncovered that 6PPD-Q considerably reduced the community diversity and altered the community assembly and functional traits of the sediment microbiome. However, we discovered that the toxicity of 6PPD-Q degradation solutions was effectively decreased, suggesting the superior detoxifying capability of the UV/PMS system for 6PPD-Q. These findings highlight the underlying detrimental impacts of 6PPD-Q on aquatic ecosystems and enrich our understanding of the photochemical oxidation behavior of 6PPD-Q.
研究领域:
环境科学
·
生态毒理学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Guoping Pan,Jia Wei,Mengdie Xu,Jiamei Li,Linhao Wang,Yanan Li,Nan Cui,Jun Li,Zhaoxu Wang
In recent years, metal-free catalysts for persulfate-mediated oxidation processes have been widely applied to remove contaminants in the aquatic environment. Herein, a simple pyrolysis approach was used to synthesize the boron doped biochars (B@TBCs) derived from boric acid mixed with tea seed shells powders. The obtained B@TBCs exhibited fantastic capability to boost PMS (0.5 mM) activation for 90%∼ removal of oxytetracycline (OTC) within 20 min. Through the correlation analysis and DFT calculations, it was concluded that the apparent rate constant of pollutants removal was greatly related to the -O-B-O- groups on the biochars, which could improve the electron-donating capacity of the biochar. In addition, the degradation process of OTC was pH-dependent because of the changed roles of ROSs under different pH. Finally, according to the DFT calculation, LC-MS and toxicological analysis, the degradation pathways of pollutants and the toxicity changes during the degradation process were obtained. These findings consolidated the theoretical basis for further boosting the catalytic activity of B-doped biochars and expanded the imagination for the modification of other metal-free biochar catalysts for PMS activation .
研究领域:
环境科学
·
催化
·
水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Zhujun Luo,Wantang Huang,Wenyan Yu,Shaoyu Tang,Kun Wei,Yuanyuan Yu,Lei Xu,Hua Yin,Junfeng Niu
Tris (2-butoxyethyl) phosphate (TBOEP) has gained significant attention due to its widespread presence and potential toxicity in the environment. In this study, the degradation of TBOEP in aquatic media was investigated using electrochemical oxidation technology . The anode Ti/SnO 2 –Sb/La–PbO 2 demonstrated effective degradation performance, with a reaction constant ( k ) of 0.6927 min −1 and energy consumption of 1.24 kW h/m 3 at 10 mA/cm 2 . CV tests, EPR tests, and quenching experiments confirmed that indirect degradation is the main degradation mechanism and ·OH radicals were the predominant reactive species, accounting for up to 93.8%. The presence of various factors, including Cl − , NO 3 − , HCO 3 − and humic acid (HA), inhibited the degradation of TBOEP, with the inhibitory effect dependent on the concentrations. A total of 13 intermediates were identified using UPLC-Orbitrap-MS/MS, and subsequent reactions led to their further degradation. Two main degradation pathways involving bond breaking, hydroxylation, and oxidation were proposed. Both Flow cytometry and the ECOSAR predictive model indicated that the intermediates exhibited lower toxic than the parent compound, resulting in a high detoxification rate of 95.9% for TBOEP. Although the impact of TBOEP on the phylum-level microbial community composition was found to be insignificant, substantial alterations in bacterial abundance were noted when examining the genus level. The dominant genus Methylotenera , representing 17.4% in the control group, decreased to 6.9% in the presence of TBOEP and slightly increased to 8.7% in the 4-min exposure group of degradation products . Electrochemical oxidation demonstrated its effectiveness for the degradation and detoxification of TBOEP in aqueous solutions, while it is essential to consider the potential impact of degradation products on sediment microbial communities.
研究领域:
环境科学
·
化学工程
·
分析化学
·
毒理学
·
微生物学
✓ 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）