PHYSICAL CHEMISTRY CHEMICAL PHYSICS
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2024
·Vol. 26
·期 44
·28266-28273
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IF 2.9
Kaihang Liu,Wenhui Ni,Qiaoyu Zhang,Xu Huang,Tao Luo,Jian Huang,Hua Zhang,Yong Zhang,Fumin Peng
The integration of photocatalysis and biological treatment provides an effective strategy for controlling antibiotic contamination, which requires precise monitoring of toxicity changes during the photocatalytic process. In this study, nanoscale TiO2 (P25) was employed to degrade tetracycline (TC) under full-spectrum irradiation, with O2 identified as a crucial reactant for the generation reactive oxygen species (ROS). The toxicity simulation results of the degradation intermediates were closely correlated with the predictions of T.E.S.T software. By analyzing the content of intermediates under different experimental conditions, we developed a machine learning model utilizing the random forest algorithm with a correlation coefficient of R2 = 0.878 and a mean absolute error of MAE = 0.02. The model can track the changes of photocatalytic intermediates, in combination with toxicity simulation, which facilitates the prediction of toxicity at different degradation stages, thus allowing selection of the optimal timing of biological treatment interventions.
研究领域:
环境科学
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化学工程
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毒理学
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机器学习
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DOI
PubMed
高影响因子
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2025
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IF 4.6
Qiaoyu Zhang,Qiao Shen,Fumin Peng,Wenjing Bian,Xu Huang,Yong Zhang,Jian Huang,Hua Zhang,Tao Luo
This study selected Doxycycline hydrochloride (DOX) as a representative antibiotic and titanium dioxide nanoparticles (P25) as a typical photocatalyst to investigate the photocatalytic degradation process. The research demonstrates three key innovations: (1) The degradation pathway of DOX by P25 was systematically elucidated through the combination of in situ reactive oxygen species (ROS) verification (confirming the dominant roles of 1 O 2 , •O 2 - , and h + ) and multi-technique intermediate tracking using liquid chromatography-mass spectrometry/two-dimensional correlation spectroscopy (LC-MS/2D-COS). This approach confirmed the direct involvement of 1 O 2 , •O 2 - , and h + in the reaction and resolved the sequence of functional group changes. (2) A random forest (RF) model was developed and integrated with T.E.S.T. simulations to construct time-resolved toxicity evolution profiles. The acute toxicity, developmental toxicity, and mutagenicity of intermediates were evaluated using the T.E.S.T. toxicity assessment software. The established RF model demonstrated high prediction accuracy with a coefficient of determination (R 2 ) of 0.932, mean absolute error (MAE) of 0.018, and root mean square error (RMSE) of 0.039. This model enables tracking of photocatalytic intermediate variations and, combined with toxicity simulation, facilitates the prediction of toxicity levels at different degradation stages, thereby deriving toxicity evolution patterns after photocatalytic degradation. (3) This study establishes a novel framework for degradation endpoint optimization through dynamic toxicity prediction, providing a strategic solution for minimizing ecological risks in photocatalytic water treatment.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jiale Lu,Amin Jv,Hongyu Zhao,Guangbo Che,Bo Feng,Yufei Zhang,Chunbo Liu,Renquan Guan
MIL-101(Cr) is an ideal material for wastewater treatment due to its large specific surface area, excellent water stability, and chemical stability. However, its limited light absorption capacity hinders its application. We loaded ferrocene carboxylic acid (Fc-COOH) onto MIL-101(Cr) by a post-synthetic modification method, which resulted in the MOF possessing excellent optical properties while maintaining its original skeleton structure. The MIL-101(Cr)/Fc-COOH (1:2), (abbreviated as CFCC-2) exhibited the best performance, achieving a removal rate of 96% for tetracycline (TC) in just 30 min. This removal rate is significantly higher compared to MIL-101(Cr) and Fc-COOH, which achieved removal rates of only 15% and 21%, respectively. We propose a possible Z-type heterojunction mechanism between MIL-101(Cr) and Fc-COOH to explain the excellent photocatalytic performance of CFCC-2. The intermediates in TC were identified using LC-MS, and the toxicity of these intermediates was predicted and evaluated through the Toxicity Estimation Software Tool (T.E.S.T.). This study provides new insights into the design and fabrication of MIL-101(Cr)-based catalysts as photodegrading organic pollutants.
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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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Junjing Li,Menghua Yin,Yu Wang,Liang Wang
In order to change the mass transfer efficiency of conventional flat plate electrodes in the catalytic process, a new filtered Pd@Ti electrode has been prepared. The results indicated that the filtered Pd@Ti electrode had the best removal efficiency of 99.59% on diclofenac (DCF) at the flux of 40.85 L/m 2 ∙h -1 . Compared to unfiltered Pd@Ti electrodes, the removal efficiency was 1.18 times higher, the current efficiency was 2.15 times higher and the cost of electricity was 69.05% lower. The electrocatalytic hydrodechlorination process of DCF by filtered Pd@Ti electrode mainly relies on indirect reductive dechlorination by H* adsorbed on the electrode surface. The removal efficiency of the filtered Pd@Ti electrode remained above 80% after six cycles. The removal mechanism and reaction pathway of filtered Pd@Ti electrode for dechlorination of different chlorinated PPCPs were proposed. Furthermore, the ecotoxicity of chlorinated PPCPs and their products were evaluated by using the toxicity estimation software tool (T.E.S.T.) model. This study confirmed the promising application of filtered Pd@Ti electrodes for the removal and detoxification of chlorinated PPCPs in wastewater.
研究领域:
环境工程
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水处理
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电化学
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毒理学
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DOI
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Yuan He,Liangjie Wang,Zhan Chen,Xia Huang,Xiaomao Wang,Xiaoyuan Zhang,Xianghua Wen
In the present study, MnMe oxide (Me = Fe, Co, Ce) were in situ embedded on the surface and inside micropores of membranes by redox reaction to fabricate novel catalytic ceramic membranes . The synergistic effect of membrane filtration and catalytic ozonation were evaluated towards atrazine degradation. MnCe-CM owned the best performance with 99.99% atrazine removal in 40 min among four catalytic membranes because of the oxygen vacancies created by Ce 3+ /Ce 4+ and Mn 2+ /Mn 3+ . MnCe-CM was subsequently chosen to explore the optimized operating conditions with a finding of ozone concentration 0.8 mg/min and pH 7. As the catalysts were successfully embedded on the surface and inside the micro-pores of MnCe-CM, the catalytic ozonation took place both on the surface and inside micropores. The reactions on the surface and inside micropores were proved very effective considering that the high specific surface provided sufficient reaction sites while the confined space facilitated the contact between •OH and the reactants. In addition, atrazine degradation pathways were proposed based on the identified byproducts. The reaction sites and the biotoxicity evaluation were calculated by density function theory (DFT) and Toxicity Estimation Software Tool (T.E.S.T), respectively. The present study provides a novel MnCe-CM with dual functions of filtration and catalytic ozonation and outlines the synergistic effect of separation and catalytic ozonation.
研究领域:
环境科学
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催化
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水处理
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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
Yuxuan He,Jin Qian,Peifang Wang,Jie Wu,Bianhe Lu,Sijing Tang,Pan Gao
The nanocomposite of MoS 2 embedded manganese ferrite doped perovskite (SrCoO 3 /MnFe 2 O 4 /MoS 2 , abbreviated as SMM) was successfully synthesized for peroxymonosulfate (PMS) activation under visible-light. It was optimized that the SMM-3 (mass ratio of MoS 2 modified nanocomposite was 0.3) exhibited excellent catalytic performance to activate PMS for levofloxacin (LVF) degradation, with the degradation efficiency of 95.1% in 20 min. Besides, SMM-3 was able to efficiently degrade LVF under real water matrix. The quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that SO 4 •- and HO • played a dominant role in reaction. Due to the photocatalytic property of nanocomposites, the visible light could excite electrons to react with oxygen and form O 2 •- , which further reacted with HO • to produce 1 O 2 . In the reaction process, the rapid redox cycle of metal ions (including Co, Mn, Fe and Mo) boosted the activation of PMS and promoted the degradation of LVF in a short time. The Density functional theory (DFT) calculation and LC-MS/MS further revealed that oxidation of piperazine ring, decarboxylation and defluorination processes were the main LVF degradation pathways. Finally, the toxicity analysis based on Toxicity Estimation Software Tool (T.E.S.T) verified the ecological risks of transformation residues.
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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光化学
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催化
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Mude Zhu,Yi Tang,Xueqin Chen,Linli Xu,Xiaoyun Fan
Constructing a chemical bond between the catalysts’ interfaces can establish a fast electron diffusion path and improve interfacial charge transport, thus produce a high efficiency in the catalytic field. We innovatively incorporate the humic acid (HA) and SrBi 2 B 2 O 7 (SBBO) to degrade oxytetracycline (OTC) under ball milling (BM), the degradation efficiency of OTC for SBBO/HA under BM is 93.17 % and its pseudo-first-order kinetic constant is 0.0434 min −1 , being 1.41 times than the sum of rate constant for HA (0.00826 min −1 ) and SBBO (0.0225 min −1 ), and 5.26 times than that for BaTiO 3 (0.00825 min −1 ), illustrating their outstanding synthetic effect of SBBO and HA on piezoelectric degradation of OTC. The mechanism of enhanced piezoelectric activity was attributed to the B-N bond which enhances the local polarized electric field improving electron transfer and contributes to the generation of •O 2 – and •OH. The possible degradation pathways involving bonds cleavage, ring-opening, and dehydroxylation process were proposed based on LC-MS and Fukui index calculation. The toxicity of intermediates generated during the piezoelectric catalysis was predicted and investigated by T.E.S.T. software and mung bean growth. This study provides a new technology of enhancing piezoelectric catalytic activity by combining HA, SBBO and BM and clarifies the mechanism in detail.
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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催化
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水处理
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Mengmeng Dou,Jin Wang,Zhaokun Ma,Boru Gao,Xue Huang
In the study, an efficient ‘1 + 1 > 2′ synergistic coupling system driven by visible light consisting of mesoporous g-C 3 N 4 (MCN) and persulfate (PS)was constructed. The free radical transformation, electron transfer and non-covalent interaction between the MCN layer and PS in the system were explored via experiments and DFT calculations. The similarity for the fate of the seven β-lactam antibiotics with typical structures in the oxidation system was studied systematically in depth. First, the consistencies and differences of the seven antibiotics were summarized from three aspects: three-dimensional structures, electron cloud distributions, and the vulnerable sites. Notably, the selective differential degradation of β-lactam antibiotics in the MCN/PS system was speculated to be related with the molecular ionization potential (MIP), as a key index to describe the difficulty of oxidation. The distribution relationship between MIP and the oxidation kinetic constant ( K ) was explored and showed the following trend: a higher MIP indicates a weaker ability to provide electrons, and this leads to a greater resistance to oxidative degradation. In total, four main oxidation pathways of β-lactam antibiotics were systematically summarized combining HPLC-QTOF-MS and the simplified Fukui function calculation. The toxicity assessment of intermediate products provided by the T.E.S.T software of USEPA also shows a decreasing trend in the oxidation process. In the end, the superior practicability and stability of the MCN/PS system was verified by complex environment simulation and cyclic test. This research clarified the selective differential degradation mechanism of β-lactam antibiotics and provided a possible idea for the effective removal of refractory organic pollutants in water.
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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药学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Yuxi Xi,Xiaojun Guo,Wei Han,Hudong Yan,Fei Zha,Xiaohua Tang,Haifeng Tian,Zhijun Zuo
The investigation about the mechanism of crystal plane regulation on the generation of oxygen vacancies remains a challenge. In this paper, BiOBr/FeMoO 4 composites were synthesized by precise control of crystal plane growth, and it exhibited the enhanced concentration of oxygen vacancies due to lower formation energy of oxygen vacancies. The composite performs higher photo-Fenton-like ability for degrading oxytetracycline hydrochloride (OTC). Structural analyses and theoretical calculations reveal that crystal plane regulation induces significant changes in oxygen vacancy concentration. The BiOBr/FeMoO 4 /peroxydisulphate (PDS) /light system, which dominated by the non-radical pathway, degraded 96.8 % ± 1.0 % of OTC within 30 min. The activation mechanism of the system and the degradation pathway of OTC were elucidated. The intermediates in the degradation process of OTC were evaluated using liquid chromatograph-mass spectrometer (LC-MS), toxicity evaluation software tool (T.E.S.T) and soybean germination experiments. This work offers novel insights into the pivotal role of crystal plane directional regulation in the quantitative generation of oxygen vacancies.
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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分析化学
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DOI
PubMed
高影响因子
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