INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Min Sun,Miao-Miao Hou,Xian-Zhang Wang,Bao-Jun Yang,Lin-Feng Zhai,Shaobin Wang
Electrocatalytic wet air oxidation (ECWAO) is a novel wet air oxidation technology using an anodic electric field to stimulate oxygen for catalytic oxidation of water pollutants at ambient condition. Herein, a mechanistic kinetic model is established based on the degradation of bisphenol A in an ECWAO process with manganese oxide (MnOx) catalysts, and the general applicability of the model is verified by triclosan degradation over a Ni@NiO catalyst and sulfamethoxazole degradation over a MnMoOx catalyst. Elementary steps involved in solid-catalyzed reaction and the assistant role of anodic electric field in the catalysis are taken into consideration. A group of kinetic equations based on the Langmuir–Hinshelwood–Hougen–Watson (LHHW) or Eley–Rideal (ER) rate laws are evaluated using the criteria of the minimization of the residual sum of squares and average error. The results show that the ECWAO reaction is best described by the LHHW model in which the surface reaction between adsorbed oxygen and adsorbed organic molecules is the rate-determining step. The key parameters controlling ECWAO reaction kinetics are the adsorption equilibrium constant of oxygen and rate constant of the surface reaction. According to the kinetic model, the reaction rates of organic pollutants are nearly linear dependent upon their concentrations within a certain range. With the increment of the circuit current, the reaction rates of organic pollutants first rise, then reach a plateau, and finally decline. The mechanistic kinetic model proves to be applicable for interpreting and predicting the ECWAO rates of organics over the transition metal oxide catalysts.
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
Surfaces and Interfaces
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2024
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IF 5.7
Donghai Wu,Hanyu Fang,Guanghua Lu,Runren Jiang,Jianchao Liu
In this study, four pharmaceutical compounds including sulfamethoxazole (SMX), oxytetracycline (OTC), ciprofloxacin (CIP), and ibuprofen (IBU) with different functional groups and p K a , were selected as representative pollutants to systematically investigate the Pharmaceutical and Personal Care Products (PPCPs) adsorption on a nanomaterial Ti 3 C 2 T x MXene in simulated solution and real surface water . The results show that Ti 3 C 2 T x was an excellent PPCPs adsorbent, but the process was affected by the characteristics of pollutants pronouncedly, the obtained maximum adsorption capacity were OTC (210.97 mg/g) > IBU (185.05 mg/g) > CIP (160.60 mg/g) > SMX (68.12 mg/g). Specially, the charge screen effect caused Ti 3 C 2 T x precipitation during CIP adsorption. The response surface methodology analysis indicates that initial solution pH (3–11) had significant effects, while the influence of humic acid (0–10 mg/L) or sodium chloride (0–10 mg/L) was limited, and the interactions between these factors was slight. In the co-adsorption process, the competitive effects reduced the adsorption of SMX and IBU, however, the enhanced positive ionization and the possible electrostatic repulsive interactions promoted that of CIP and OTC. In real surface water, although the influence of natural organic matters was negligible, the preferential adsorption of background metal ions such as aluminum and calcium ions reduced the adsorption capacity of the selected PPCPs by approximately 29.9 % to 88.4 %. Moreover, the adsorbent characterization conjoined with performance examination imply that electrostatic attraction dominated the Ti 3 C 2 T x adsorption of PPCPs, and hydrogen bonding interactions as well as surface complexation might also contributed. These observations suggest that Ti 3 C 2 T x MXene has the potential for use as adsorbent to eliminate aqueous PPCPs, nevertheless, the interference of co-existing metal ions and the stability of adsorbent were also noteworthy.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jilong Wang,Qi Xiang,Ye Han,Zeyu Ma,Wei Cheng,Jie Sun,Shaobin Wang
To overcome the limitations of traditional Electro-Fenton (EF) in natural waters, such as low conductivity and metal ion leaching, we developed a novel metal-free EF system incorporating solid polymer electrolytes (EF-SPE). Nitrogen-doped carbon cathodes, optimized via calcination (e.g., 800 °C), enabled efficient in-situ H 2 O 2 electro-generation and activation for carbamazepine (CBZ) degradation. This EF-SPE system achieved a CBZ degradation half-life of 10 min (k = 0.052 min −1 ), operated effectively across a broad pH range (3–9), and exhibited low specific energy consumption for mineralization (6.73 kWh·m −3 ). Experimental and computational studies reveal that graphitic N and pyridinic N were the primary active sites for the electro-generation of H 2 O 2 and its activation to •OH, respectively. The system demonstrated universal efficacy for various pharmaceuticals and personal care products in different natural waters, showcasing its potential for sustainable water purification.
研究领域:
环境科学
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水处理技术
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电化学
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材料科学
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污染物降解
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可持续技术
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DOI
高影响因子
Journal of Environmental Chemical Engineering
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2023
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IF 7.7
Zhengqiaoruo Zhu,Nan Zhou,Yakun Li,Linlin Zhang
In this study, a novel Fe, S, P co-doped g-C 3 N 4 photocatalytic nanoreactor was successfully synthesized. The unique structure of Fe, S, P co-doped g-C 3 N 4 enhances its optical absorption , and there are plenty of active sites and photogenerated carrier separation. Consequently, the Fe, S, P co-doped g-C 3 N 4 demonstrated excellent photocatalytic-Fenton degradation activities under visible light irradiation. Remarkedly, 5 mg/L of sulfamethazine (SMZ) is completely photocatalytic-Fenton degraded following 25 min under visible light irradiation. It further shows that·O 2 - plays a crucial part in the photocatalytic-Fenton process, leading to the decomposition of sulfamethazine. The decline of Bisphenol A (BPA) further demonstrates that this photocatalytic-Fenton system can be effectively used to remediate pharmaceutical and personal care product contamination in environmental waterways.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Jie Mao,Jihui Wang,Jun Zhang,Sha Shi,Yizhen Zhang,Yaohui Bai,Jiuhui Qu
The persistence of pharmaceuticals and personal care products (PPCPs) in aquatic ecosystems poses severe environmental risks, primarily owing to their incomplete removal by conventional treatment methods and potential for inducing bacterial resistance. While CdS/g-C 3 N 4 heterojunctions exhibit promise for photocatalytic degradation, the role of nitrogen-defect engineering in steering interfacial charge behavior to synergize photocatalysis with persulfate (PS)-based advanced oxidation remains unexplored. Herein, a nitrogen-deficient Z-scheme CdS/g-C 3 N 4 (CdS/N-CN) heterojunction was designed via hydrothermal synthesis to enable solar-driven cooperative photocatalysis and PS activation for PPCPs degradation. The optimized system achieved complete degradation of 10 mg/L sulfamethoxazole (SMX) within 60 min under visible light, achieving a rate constant (0.157 min −1 ) 29 times higher than pristine g-C 3 N 4 . Mechanistic investigations demonstrated dual-pathway operation: a built-in electric field drove Z-scheme charge transfer, migrating electrons from N-CN to CdS while holes in N-CN served as primary oxidants. Meanwhile, electrons from CdS activated PS to generate sulfate and hydroxyl radicals, with the latter transforming into singlet oxygen for supplementary oxidation. This synergistic photocatalysis-PS activation system maintained efficient redox activity while enhancing charge separation, ultimately enabling effective PPCPs decontamination. This research presents a novel strategy for leveraging solar-driven heterojunctions and persulfate chemistry for sustainable water remediation.
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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水处理技术
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光催化
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高级氧化工艺
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产品关联
DOI
高影响因子
Analytical Methods
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2025
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IF 2.6
Rongting Zhuo,Rong Bao,Yanzhong Fan,Qi Lin,yan yang
Residues of pharmaceuticals and personal care products (PPCPs) in drinking water pose significant public health risks. To assess these residues in water, this study developed a solid-phase extraction combined with ultra-performance liquid chromatography-tandem mass spectrometry method (SPE-UPLC-MS/MS) for the simultaneous quantitative determination of 98 PPCP residues in drinking water. By optimizing the pretreatment method and analysis conditions, the method exhibits excellent linearity, with all PPCPs showing correlation coefficients (R²) greater than 0.99 within the concentration range of 0-100 μg/L. Recovery rates ranged from 60.7% to 119.0%, and the relative standard deviations (RSDs) below 20%. The limits of detection (LODs) were between 0.034 and 4.001 ng/L. Residues such as amisupride and 1,7-dimethylxanthine were detected in water samples. This method is simple, sensitive, and suitable for high-throughput detection of trace PPCPs in drinking water, providing reliable technical support for water quality monitoring.
研究领域:
环境科学
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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 ENVIRONMENTAL SCIENCE AND HEALTH PART A-TOXIC/HAZARDOUS SUBSTANCES & ENVIRONMENTAL ENGINEERING
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2019
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IF 1.536
Xiaofeng Wang,Beihai Zhou,Xia Shao
Dimethylamine-based pharmaceutical personal care products (DMA-based PPCPs) are a group of N-nitrosodimethylamine (NDMA) precursors. The acid dissociation constant (pKa) values of four DMA-based PPCPs were determined by potentiometric titration over the pH range of 3–11. The pKa values of ranitidine, nizatidine, doxylamine and carbinoxamine corresponding to the DMA moiety were 8.4, 6.8, 9.4 and 9.1, respectively. Competition reaction kinetics and pseudo-first-order reaction kinetics were used to determine the reaction rate constant (k) of the DMA-based PPCPs with O3, NaClO, ClO2 and KMnO4. Comparing the degradation rate constants of the four DMA-based PPCPs, the results of ClO2 oxidation were close, and for the other three oxidants, the order was kranitidine ≈ knizatidine > kdoxylamine ≈ kcarbinoxamine. Comparing the reaction rate of the four oxidants, for ranitidine and nizatidine, the order was kNaClO > kO3 > kKMnO4 > kClO2, and for doxylamine and carbinoxamine, the order was kO3 > kNaClO > kClO2 > kKMnO4.
研究领域:
环境科学
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化学动力学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2016
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IF 3.299
Ning Zhuo,Yaqian Lan,Weiben Yang,Zhen Yang,Xiaomin Li,Xia Zhou,Yang Liu,Jiachun Shen,Xuntong Zhang
Porous metal-organic frameworks (MOFs) have great potential as high-effective adsorbents for water treatment. However, poor separability restricts their practical application. To overcome the drawback, both MIL-101(Cr)/sodium alginate (MIL-101(Cr)/SA) and MIL-101(Cr)/chitosan (MIL-101(Cr)/CS) composite beads were prepared and characterized. Adsorption of three selected pharmaceuticals and personal care products (PPCPs) (benzoic acid (BEN), ibuprofen (IBU) and ketoprofen (KET)) onto the two composite beads was investigated and compared with pristine SA and CS beads. Kinetic plots, pH dependence, isotherm data, and influences of ionic strength were reported. The MIL-101(Cr)/CS beads exhibit much higher adsorption capacity than SA, CS and MIL-101(Cr)/SA, and the adsorption amounts of three PPCPs onto MIL-101(Cr)/CS follow the order of KET > IBU > BEN. The adsorption amounts of the three PPCPs on the MIL-101(Cr)/CS increased quickly during the first 60 min of contact time and then achieved the adsorption equilibrium after ∼180 min. Not only the protonated amine groups but also the Cr center of the adsorbents exerted electrostatic attraction with the deprotonated carboxyl groups of contaminants, as elucidated by X-ray photoelectron spectroscopy (XPS). Based on the adsorption isotherms and π-energy analysis of three PPCPs, π-π interaction of aromatic groups between adsorbents and contaminants also contributed to the adsorption. The MIL-101(Cr)/CS beads exhibited good regenerability over several repeated adsorption/desorption cycles. Overall, this study is believed to enlarge the application of MOFs on the removal of emerging contaminants from waters.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CERAMICS INTERNATIONAL
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2023
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IF 5.2
Kai Xuan,Taiguang Li,Yongmei Hao
Adequate separation of photogenerated carriers plays an important role in the photocatalytic degradation of pollutants. Here, a noble-free spatially separated photocatalyst rGO-CdS-MnO x (GCM) has been designed for removing environmental pollutants efficiently. rGO and MnO x are employed as the collectors of photoinduced electrons and holes, respectively. Under light irradiation, the electrons and holes motivated by CdS can directionally transfer to the rGO and MnO x , leading to the exposure of both reduction and oxidation surfaces, thereby enhancing the photocatalytic activity. Our results demonstrated that GCM-30 can remove 86.56 % of carbamazepine and 95.83 % of tetracycline hydrochloride within 30 min and 15 min, respectively, and 95.49 % of Cr (VI) within 21 min. Our work demonstrates that this dual functional photocatalyst may provide new strategies for the spatially separated photocatalysts for removing environmental pollutants.
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产品关联
DOI
高影响因子
AQUATIC TOXICOLOGY
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2021
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IF 4.964
Naima Hamid,Muhammad Junaid,Rakia Manzoor,Jin-Jing Duan,Ming Lv,Nan Xu,De-Sheng Pei
Pharmaceuticals and personal care products (PPCPs) as emerging contaminants are ubiquitously present in the aquatic environment. Using in vivo and in silico techniques, this study aims to elucidate tissue distribution and endocrine disruption effects of chronic exposure (120 days) to PPCP mixture at environmentally relevant concentrations (ERCs) in adult zebrafish. Results from UHPLC-MS/MS analyses showed elevated distribution of PPCPs in zebrafish tissues in the order of liver > gonad > brain. Upregulation of steroid hormone receptors, both gonadotropin, and steroidogenic genes perturb the HPG axis pathway in females, while male fish exhibited significantly downregulated expressions of vtg, cyp17 , and 17βhsd genes with inhibited fecundity. The Spearman correlation indicated a significant positive relationship between PPCPs bioaccumulation and mRNA levels of HPG axis genes. In silico molecular docking (MD) revealed specific amino acid residues of PPCPs binding with zebrafish estrogen receptors. Furthermore, the strongest binding energies of sulfamethoxazole, carbamazepine, and triclosan were discovered in erα and erβ estrogen receptors, confirming PPCPs' xenoestrogenic behavior. To summarize, chronic exposure to ERCs resulted in a high accumulation of PPCPs in the liver and gonad tissues of adult zebrafish, as well as associated perturbed genetic responses. As a result, strict environmental regulations for the disposal of PPCPs should be ensured to protect ecological and public health.
研究领域:
环境科学
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毒理学
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水生生物学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
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IF 5.1
Junjing Li,Ying Zhang,Yiqi Liang,Liang Wang,Bo Li,Fei Shao
Pharmaceuticals and personal care products (PPCPs) are refractory emerging organic pollutants, and clofibric acid (CA) is a typical poorly biodegradable representative. Herein, a nitrogen-doped carbon nanotube (N-CNT) tubular ceramic membrane electrode was fabricated for electro-activated peroxymonosulfate (EA-PMS) degradation of CA, with systematic optimization of preparation and operational conditions. Nitrogen doping introduced pyrrolic/graphitic N active sites and increased structural defects, while the tubular configuration intensified mass transfer. The optimized electrode achieved > 90% CA removal within 30 min, maintained > 95% efficiency over 11 cycles, and exhibited broad-spectrum degradation for typical PPCPs, with low EE/O (0.0417 kWh m -3 order -1 ) and high PMS utilization (84.3%). Singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen species, driving CA degradation via synergistic radical/non-radical oxidation. Three CA degradation pathways were elucidated by HPLC-MS, and ECOSAR simulations confirmed reduced aquatic toxicity of its intermediates. This work develops a high-performance EA-PMS electrocatalytic membrane system, providing a scalable platform for advanced treatment and risk control of trace PPCPs in water.
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Junjing Li,Xingzhou Mu,Di Wu,Ganhua Liu,Liang Wang
The development of efficient electrochemical coupling systems for persulfate activation is crucial for expanding the treatment of pollutants such as pharmaceuticals and personal care products (PPCPs) in wastewater. In this study, we present an electrically activated persulfate-coupled N-doped graphene membrane electrode system, which achieves complete (100 %) removal of chlortetracycline hydrochloride (CTC) within 90 min. Nitrogen doping significantly enhances the catalytic activity of graphene membrane electrodes for PMS activation, improving CTC degradation by 45 %. X-ray photoelectron spectroscopy (XPS) identified pyridinic nitrogen and graphitic nitrogen as the dominant PMS-active sites. Free radical quenching experiments and electron spin resonance (ESR) spectroscopy elucidated the reaction mechanism. Under an external electric field, the N-doped graphene membrane electrode functions as an anode, triggering PMS activation and generating reactive oxygen species (ROS), including SO 4 •- , •OH and 1 O 2 . Furthermore, high-performance liquid chromatography-mass spectrometry (HPLC-MS) was employed to analyze intermediate products and assess the toxicity of CTC. The system exhibited excellent pH adaptability and broad applicability for PPCPs removal. This innovative electrochemical coupling system with N-doped graphene membrane electrodes advances the prospects of electrochemical technology in water pollution control. Environmental Implication In this study, we propose an innovative “electrochemically activated persulfate coupled N-doped graphene membrane electrode system” strategy. Using this strategy, we successfully fabricated a graphene membrane electrode material with N-active sites for persulfate activation. The N-sites in this structure enhance the charge distribution, electronic density, and spin density of the graphene material, thereby facilitating the activation of persulfate. The electrode material not only exhibits facile synthesis, excellent activity, and high stability, but also demonstrates considerable promise for applications in the field of environmental remediation.
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产品关联
DOI
高影响因子