WATER RESEARCH
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2022
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IF 13.4
Fuwei Sun,Tianhu Chen,Ziyang Chu,Peixun Zhai,Haibo Liu,Qiang Wang,Xuehua Zou,Dong Chen
A system of Cu 2+ /calcite/PDS was constructed to degrade sulfadiazine (SDZ). Different from the traditional Cu-mediated activation, a low concentration of Cu 2+ that met drinking water standards (≤ 1 mg/L) transformed into Cu(Ⅱ) solid in the presence of calcite, and then enhanced the degradation of SDZ via PDS activation over a pH range from 3 to 9. According to scavenger and chemical probe experiments, Cu(Ⅲ), rather than radicals (hydroxyl radicals and sulfate radicals) and singlet oxygen, was the predominant reactive species, which was responsible for the degradation of SDZ. Based on the results of XRD, ATR-FTIR, and CV curves et al., CuCO 3 was the main complex with high reactivity for PDS activation to form Cu(Ⅲ). Moreover, detailed degradation pathways of sulfadiazine were proposed according to the UPLC-ESI-MS/MS and their toxicity was predicted by ECOSAR. Besides, the real water matrix would not seriously affect the degradation of SDZ in the Cu 2+ /calcite/PDS system. In summary, this study reveals a new insight into the synergistic effect of Cu 2+ and calcite on the SDZ degradation, and promotes an understanding of the environmental benefits of natural calcite.
研究领域:
环境科学
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化学工程
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分析化学
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水处理
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 30
·75595-75609
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IF 5.8
Jiang Mengyun,Xu Zhongjun,Zhang Tingting,Zhang Xirong,Liu Ying,Liu Peng,Chen Xiaochun
In this work, FeS supported SBA-15 mesoporous silica catalyst (FeS@SBA-15) was synthesized successfully, characterized and first applied to persulfate (PS) activation for the degradation of imidacloprid in wastewater. The as-prepared 3.5-FeS@SBA-15 presented an impressive imidacloprid removal efficiency of 93.1% and reaction stoichiometric efficiency (RSE) of 1.82% after 5 min, ascribed to the synergetic effects of improved FeS dispersion and abundant surface sites by SBA-15. Electron paramagnetic resonance spectra and quenching experiments proved that both SO 4 ·- and ·OH were produced in FeS@SBA-15/PS system, and SO 4 ·- played a dominant role in the degradation process. The S 2- can accelerate the cycling of Fe(III)/Fe(II) during activation and increase the steady-state concentration of Fe(II). More importantly, the constructed heterogeneous system exhibited an efficient and stable catalytic activity over a wide range of pH (3.0-9.0), temperature (283K-313K), inorganic ion (NO 3 - ) and humic acid (1-20 mg/L). Moreover, the density functional theory calculations were conducted to predict the potential reaction sites of imidacloprid. Based on eighteen identified intermediates, four main degradation pathways were proposed: hydroxylation, dechlorination, hydrolysis, and the ring cleavage of the imidazolidine. ECOSAR analysis indicated hydroxylation and dechlorination played a key role in the detoxification of the formed compounds. These findings would provide new insights into the application of FeS@SBA-15 catalyst in wastewater treatment and the removal mechanism of imidacloprid from wastewater.
研究领域:
环境科学
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催化
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废水处理
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化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL POLLUTION
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2023
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IF 8.9
Linli Dai,Yi Xie,Yongkui Zhang,Yabo Wang
Metal-free carbon catalysts perform well in peroxymonosulfate-based advanced oxidation process for the treatment of organic pollutant-containing wastewater. Herein, a natural biomolecule of adenosine triphosphate (ATP), containing abundant N and P elements, served as sole precursor to prepare N,P-co-doped carbon through one-step anoxic pyrolysis , which was applied as peroxymonosulfate activator to treat bisphenol-contaminated water. Owing to the endogenous N and P elements in ATP, in-situ doping was achieved for the prepared carbon material with excellent doping effect, such as high doping amount and numerous defects. During pyrolysis process, the generated gases facilitated the exfoliation of carbon structure, resulting in a nanosheet-like morphology with large specific surface area, e.g., 852.75 m 2 g −1 for NPCN-900 sample obtained at 900 °C. Benefiting from the structural modulation brought by N,P co-doping, typical sample of NPCN-900 presented excellent catalytic performance towards bisphenol AF (BPAF) degradation through PMS activation . An apparent reaction rate constant of 0.4115 min −1 was calculated under the investigated reaction conditions. Further studies indicated that 1 O 2 , surface-bound •OH and SO 4 − • worked together in NPCN-900/PMS system for BPAF degradation. Graphitic N, pyrrolic N, C O groups, defect structure and the doped P atoms in NPCN-900 contributed to PMS activation. It was also important that the toxicity of BPAF solution could be preliminarily eliminated after treatment by NPCN-900/PMS system, which was verified by ecotoxicity assessments through ECOSAR program and green algae growth experiments.
研究领域:
环境科学
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材料科学
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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
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Mian Li,Lian-Yu Qiu,Tian-Yang Zhang,Bin Xu,Dan Yang,Ting Ye,Heng Luo
Advanced oxidation processes (AOPs) based on Fe 2+ /persulfate (PS) have been widely applied in water treatment but face critical challenges: inefficient radical utilization due to excess Fe 2+ scavenging, unsustainable reactivity from irreversible Fe 2+ -to-Fe 3+ conversion, and ambiguous dominant reactive species (e.g., SO 4 − / OH vs. high-valent iron). Ferric oxalate complexes address these limitations by enabling light-driven iron photoreduction and the Fe 2+ /Fe 3+ cycle. However, direct comparisons of degradation efficiency, mechanisms, and environmental risks between Fe 2+ /PS and UV/Fe(C 2 O 4 ) 3 3− /PS remain scarce. Using iohexol as a model, this study directly compared the two systems. The UV/Fe(C 2 O 4 ) 3 3− /PS system achieved 98.8 % iohexol degradation in 60 min (vs. 69.9 % for Fe 2+ /PS) and reduced iron sludge by 70–80 %. Both systems relied on SO 4 − and OH, but UV/Fe(C 2 O 4 ) 3 3− /PS enhanced radical yield via photocatalytic iron cycling, whereas Fe 2+ /PS depended on Fe(IV). In Fe 2+ /PS, contributions were Fe(IV) (29.4 %) > SO 4 − (25.9 %) > OH (20.2 %); in UV/Fe(C 2 O 4 ) 3 3− /PS, SO 4 − (63.6 %) > OH (23.7 %) > Fe(IV) (23.7 %). Electrical energy per order (EE/O) analysis showed UV/Fe(C 2 O 4 ) 3 3− /PS consumed 1.166 kWh mM −1 , 60.2 % lower than Fe 2+ /PS (2.524 kWh mM −1 ). Acute toxicity tests with Vibrio fischeri exhibited 67.7 % inhibition in Fe 2+ /PS, significantly higher than 36.4 % in UV/Fe(C 2 O 4 ) 3 3− /PS. Ecological Structure-Activity Relationships (ECOSAR) modeling and disinfection by-products (DBPs) risk assessment further confirmed lower risks in UV/Fe(C 2 O 4 ) 3 3− /PS, with 50 % lethal concentration ((LC 50 ) for aquatic organisms 2.3-fold higher and genotoxicity potency 41.7 % lower than Fe 2+ /PS. These results bridge the efficiency-risk gap between the two systems and offer a three-dimensional (efficiency-cost-safety) framework for AOP selection.
研究领域:
环境工程
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水处理
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化学氧化
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毒理学
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自由基化学
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污染控制
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高级氧化工艺
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能源效率
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产品关联
DOI
高影响因子
WATER RESEARCH
·
2021
·
IF 11.236
Lixiao Wang,Yajie Zheng,Yiran Zhou,Junhe Lu,Jean-Marc Chovelon,Yuefei Ji
Ketoprofen (KTF) is a nonsteroidal anti-inflammatory drug frequently detected in natural and engineering waters. Because KTF is particularly photolabile (half-life ∼4 min), knowledge of the fate and ecological risks of KTF photoproducts in the aquatic environment is especially essential. Herein, we systematically investigated the photophysics, photochemistry , and photosensitization of KTF photoproducts in aqueous solution under 365 nm irradiation (UV 365 ). Results show that KTF photolyzed rapidly and formed 3-ethyl- α -hydroxylbenzophenone (EtOH-BP), 3-ethyl- α -hydroperoxylbenzophenone (EtOOH-BP), 3-acetylbenzophenone (AcBP), and 3-ethylbenzophenone (EtBP), as identified by liquid chromatography-tandem mass spectrometry (LC-MS/MS) and high-resolution mass spectrometry (HRMS). The presence of O 2 significantly affected the evolution of photoproducts during KTF photolysis. The photophysical properties of EtBP and AcBP were characterized by spectroscopic approaches. In particular, transient absorption spectra obtained by nanosecond laser flash photolysis (LFP) indicated that EtBP and AcBP were excited to triplet states with lifetimes of 28 and 2.4 µs, respectively. EtBP underwent further photodegradation , giving rise to EtOH-BP, EtOOH-BP, and AcBP upon UV 365 irradiation. The reaction is proposed to proceed through an excimer precursor ( 3 [EtBP···EtBP]*) followed by intramolecular H-abstraction. In contrast, AcBP was relatively photostable, particularly under aerated condition. Both EtBP and AcBP have strong photosensitizing activity, as evidenced by the triplet probe 4-( N,N -dimethylamino)benzonitrile (DMABN). ECOSAR program suggested that the photoproducts are more ecotoxic and bioaccumulative than the parent KTF. Results of this study underscore the need to scrutinize the formation and fate of KTF photoproducts in sunlit surface waters.
研究领域:
环境科学
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光化学
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毒理学
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分析化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jiahao Lai,Peng Xiao,Yafei Li,Shihai Cui,Jing Yang,Hongzhen Lian
Broadening the light absorption and inhibiting carrier's recombination are vital to the improvement of photocatalytic performance. Herein, self-assembly 3D hierarchical microsphere BiOIO 3 /Bi 5 O 7 I Z-scheme heterojunction with carrier transfer channel was firstly fabricated by in-situ solvothermal method. The degradation efficiency for bisphenol A (BPA) reached 98.9 % within 60 min visible light irradiation. The enhanced photocatalytic activity was benefited from the Z-scheme system assisted by iodate/iodide (IO 3 - /I - ) as carrier transfer channel that not only accelerated the interfacial charge separation, but also provided massive reactive centers for obtaining high redox capacity. The vulnerable sites and the degradation pathways of BPA were identified by density functional theory calculations and liquid chromatography-mass spectrometry analyses. The toxicity of BPA and its intermediates were predicted by ECOlogical Structure Activity Relationship (ECOSAR) and the results demonstrated that BPA was eventually mineralized to harmless products. The Z-scheme charge transfer mechanism was deeply elucidated based on the role of active species (·O 2 - , ·OH and h + ), band structure and carrier separation efficiency. This study provides a promising strategy for the photoactivity enhancement of bismuth based heterojunction in environment purification.
研究领域:
环境科学
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材料科学
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化学
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光催化
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毒理学
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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
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化学工程
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分析化学
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毒理学
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微生物学
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产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Chao Qu,Na Ren,Shu-jun Zhang,Yan-gang Li,Shu-juan Meng,Xiao-hu Li,Shan-quan Wang,Da-wei Liang,An-ran Li
Triclosan (TCS) is an emerging contaminant that threatens the environment and human health. This study was conducted to investigate TCS abatement by a novel electro-oxidation (EO) process, which used a Ti-based nickel and antimony doped tin oxide (NATO/Ti) anode and a carbon nanotubes (CNTs) doped carbon/PTFE (CNTs-C/PTFE) gas diffusion electrode (GDE) for oxygen reduction reaction (ORR). A comparative study was also performed for TCS degradation by using a traditional EO with a nickel foam cathode, termed as HER-EO. The optimal initial TCS concentration, current density and solution pH for TCS degradation during the ORR-EO and HER-EO were investigated. Results showed that ORR-EO removed more than 98% of TCS in 10–60 min under the concentration of 5–50 mg/L. The TCS degradation followed pseudo-first-order kinetics and its main intermediates were observed during the ORR-EO and HER-EO using liquid chromatography combined mass (LC-MS). The results of FED analysis and toxicity prediction by ECOSAR software showed that less intermediates accumulated during the ORR-EO and the residues were less harmful. The ORR-EO degradation mechanism for TCS was attacking on the ether bond and the benzene ring by • OH. This novel ORR-EO process exhibits a great merit in the field of emerging contaminants abatement.
研究领域:
环境科学
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化学工程
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水处理
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电化学
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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）