JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Xukai Li,Weirui Chen,Dongpo Liu,Gaozu Liao,Jing Wang,Yiming Tang,Laisheng Li
Due to its low interfacial electron migration ability and highly hydrophilic, Fe-MCM-41 (FeM) had poor activity and stability during catalytic ozonation . To this end, the secondary metal Zn and Si-F group were introduced into the framework of FeM to create surface potential difference and hydrophobic sites. Comparative characterizations showed that there existed rich acid sites with great potential difference on F-Fe-Zn-MCM-41 (FFeZnM). Additionally, because of the existence of hydrophobic and electron-withdrawing Si-F unit, the electron migration ability, hydrophobicity and acidity of FFeZnM were enhanced. The greater O 3 mass transfer was induced by Si-F group and O 3 was directly activated at Fe and Zn Lewis acid sites into •OH, •O 2 - and 1 O 2 . With •OH acting as main species, FFeZnM/O 3 achieved the superior IBP removal (93.4%, 30 min) and TOC removal (46.6%, 120 min) over those of sole O 3 and F-FeM/O 3 processes, respectively. HCO 3 - , Cl - , NO 3 - and SO 4 2- hindered IBP degradation by FFeZnM/O 3 , but high concentration humic acid (HA) exhibited promotion by forming HA-IBP complex. IBP degradation by FFeZnM/O 3 was enhanced with tap water , river water, and effluent from the secondary sedimentation tank of the sewage plant acting as medium. This study proposed an innovative approach to catalyst design for catalytic ozonation.
研究领域:
环境科学
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材料科学
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PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2018
·
IF 4.61
Yang Yu,Fei Huang,Yide He,Xiyang Liu,Chenjing Song,Yanhua Xu,Yongjun Zhang
In this study, heterogeneous Fenton-like degradation of ofloxacin (OFX) was investigated by sludge derived carbon (SC). The effects of SC catalyst, temperature and pH on the efficiency of ofloxacin degradation were investigated. SC treated with sulfuric acid (SC-H 2 SO 4 ) performed high catalytic activity , indicating that sulfate group produced low pH of the surface and was beneficial for heterogeneous Fenton-like degradation. The removal of ofloxacin and TOC was 91.5% and 62.3%, respectively, after 180 min adsorption and 540 min oxidation, at pH 6 and a dosage of 138 mg L −1 H 2 O 2 . It was found that OFX conversion increased with the decrease of pH and OFX was degraded under the wide range of pH (3–6) by SC-H 2 SO 4 . These promising results clearly demonstrate the potential of the heterogeneous Fenton-like process for the effective degradation of ofloxacin by SC-H 2 SO 4 . Based on intermediated products identified by gas chromatography–mass spectrometry, a possible OFX oxidation pathway in Fenton-like reaction was proposed.
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
·
2024
·
IF 8.1
Xu Yin,Jie Zhang,Siru Chen,Wei Li,Hongwei Zhu,Kajia Wei,Yonghao Zhang,Haoming Chen,Weiqing Han
In this work, an electric field-enhanced heterogeneous catalytic ozonation (EHCO) was systematically investigated using a prepared FeOx/PAC catalyst. The EHCO process exhibited high sulfadiazine (SDZ) and TOC removal efficiency compared with electrocatalysis (EC) and heterogeneous catalytic ozonation (HCO) process. Almost 100% of SDZ was removed within 2 min, and the TOC removal reached approximately 85% within 60 min. Quenching experiments and EPR analysis suggested that the prominent SDZ and TOC removal performance is supported by the enhanced ·OH generation ability. Further study proved that H 2 O 2 formed by O 2 electrochemical reduction, peroxone reaction and electrochemical reduction of ozone contributed to improving ·OH generation. Furthermore, the EHCO system showed satisfactory stability and recyclability compared to conventional HCO systems, and the SDZ and TOC removal rates were maintained at ≥95% and ≥70% in 16 consecutive recycles, respectively. Meanwhile, XPS analysis and Boehm's titration for the FeOx/PAC catalyst used in HCO and EHCO process confirmed that the external electron supply could restrain the oxidation of surface functional groups of PAC and maintain a balance of the Fe(II)/Fe(III) ratio, which proved the critical role of cathode reduction in catalyst in situ regeneration during long consecutive recycles. In addition, the EHCO system could achieve more than 80% SDZ removal within 2 min in different water matrices. These results confirmed that the EHCO process has a wide application perspective for refractory organics removal in actual wastewater.
研究领域:
环境科学
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催化化学
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水处理工程
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
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2020
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IF 7.183
Songxue Wang,Jiayu Tian,Linran Jia,Jialin Jia,Sujie Shan,Qiao Wang,Fuyi Cui
CuO catalyst dispersed in the feed water (CDF) and CuO catalyst immobilized on the ceramic hollow fiber membrane (CIM) for peroxymonosulfate (PMS) activation were developed and employed in the submerged membrane filtration systems for drinking water treatment , respectively. The performance of the CDF and CIM systems was systematically investigated and compared. The result indicated that BPA concentration, PMS dosage and CuO content exerted much less influence on BPA degradation in the CIM system as compared with that in the CDF system. The CIM system exhibited a greater advantage in the performance of BPA degradation and TOC removal when treating a large volume of feed (>300 mL). In addition, the effect of actual water matrix on the two systems was evaluated. The CIM system showed higher resistance to the adverse influence and better anti-fouling performance than the CDF system. The comparative study on the performance of CDF and CIM systems provides meaningful information for developing the process of membrane filtration coupled with PMS oxidation .
研究领域:
环境科学
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水处理工程
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DOI
高影响因子
Journal of Water Process Engineering
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2019
·
IF 3.173
Senlin Ma,Xingtao Zuo,Juan Xiong,Cong Ma,Zhongbing Chen
An ozonation process combined with hydrophobic adsorbent high silica ZSM-5 (HSZSM-5) was designed to enhance sulfamethoxazole (SMX) removal and reduce the ozone consumption. The promoted effect of HSZSM-5 on SMX removal was investigated in terms of SMX removal and TOC removal efficiency as well as the ozone consumption. The impacts of pH and CO 3 2− /HCO 3 - were also analyzed. The presence of HSZSM-5 helped to increase the SMX degradation and TOC removal efficiency and their kinetics rate constants. HSZSM-5 adsorption behaviors for SMX and its degradation intermediates were responsible for the findings. Direct ozone oxidation was the main mechanism of SMX removal as HZSM-5 could not contribute to producing H 2 O 2 and •OH. Much higher CO 3 2− /HCO 3 - concentration (≥10 mM) and pH value (>7) were in favor of SMX degradation. HSZSM-5 had a positive contribution to SMX removal. The mass ratio of ozone consumption to the removed SMX reduced to 0.63 g O 3 /g SMX. This system of introducing high silica zeolite in the ozonation/adsorption process is an environmentally and economically sound technology to removal micropollutants.
研究领域:
环境科学
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水处理技术
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Ge Song,Xuedong Du,Yang Zheng,Pei Su,Yunping Tang,Minghua Zhou
To promote the reduction of Fe 3+ and improve the mineralization of organic pollutants , a novel electro-Fenton coupled with sulfite (Fe 3+ -EF/sulfite) process was constructed, which was superior to Fe 3+ -EF process in terms of carbamazepine (CBZ) degradation and mineralization with 5.99 times enhancement in degradation rate constant and 15.7 times enhancement on TOC removal. The complexation of Fe 3+ and sulfite prevented the precipitation of Fe 3+ , reduced Fe 3+ to Fe 2+ , and accelerated the iron cycle, so that H 2 O 2 utilization efficiency (0.051 mg TOC mg H2O2 −1 ) was greatly improved and electric energy consumption was greatly reduced (0.081 kWh g −1 TOC). The quenching experiments and EPR test confirmed that the reactive species, such as SO 3 •- , SO 4 •- , • OH, O 2 •- and 1 O 2 were responsible for the degradation of CBZ. This process also expanded the pH application range from 3 to 9 with satisfactory CBZ removal efficiency. This work verified the suitability of the Fe 3+ -EF/sulfite process for different sulfites (sulfite and bisulfite), typical pollutants (atrazine, sulfamethazine, rhodamine B) and real wastewater with 2.1–18.7 folds enhancement in degradation rate. The Fe 3+ -EF/sulfite process can achieve deep mineralization with low cost and simple operation, which has a broad and cost-effective application prospect in removal of refractory organic pollutants.
研究领域:
环境科学
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水处理技术
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DOI
PubMed
高影响因子
CHEMOSPHERE
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2019
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IF 5.108
Chengzhi Zhou,Yanping Wang,Jie Chen,Lei Xu,Haiming Huang,Junfeng Niu
Electrochemical degradation of antiviral drug abacavir was investigated by using a penetration flux porous Ti/SnO 2 –Sb anode prepared by sol-gel method. The effects of applied current density, initial pH, and inorganic anions on the degradation kinetics were systematically studied. Degradation efficiency more than 97% was performed in only 10 min at a current density of 0.2 mA cm −2 . The corresponding degradation rate constant and the lowest electrical energy per order were calculated to be 0.36 min −1 and 6.5 mWh L −1 , respectively. Extending the reaction duration to 5 h, 53.3% of TOC removal was observed. The results indicated that effective degradation of abacavir appeared in the penetration flux porous Ti/SnO 2 –Sb anode with a very low energy consumption. Furthermore, the electrochemical intermediate products and the reaction site during abacavir degradation were detected and recognized. The quantitative structure-activity relationship model revealed that the potential risks of abacavir to the aquatic organism, such as fish, greatly decreased after flowing through the penetration flux porous Ti/SnO 2 –Sb anode.
研究领域:
环境科学
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药学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Jiang Lu,Jingxiang Sun,Xixi Chen,Shuanghong Tian,Dingsheng Chen,Chun He,Ya Xiong
Herein a novel coupling process of simultaneous catalytic ozonation and photocatalysis (SCOP) using a bifunctional catalyst for the antibiotics wastewater treatment was developed. MgMnO 3 , as the first example of bifunctional catalyst, was successfully prepared by a simple sol-gel method. In the MgMnO 3 -mediated SCOP process, the TOC removal of sulfamethoxazole, tetracycline, ciprofloxacin, and trimethoprim within 80 min reached 94.7 ± 0.9%, 88.4 ± 0.9%, 97.8 ± 1.0%, and 76.3 ± 0.9%, respectively, much higher than that in ozonation or photocatalysis (less than 20%). The first order kinetics reaction constant of TOC removal in the case of tetracycline degradation by SCOP is 2.58 × 10 −2 min −1 , which is 2.7, 23.0, and 6.2 times that by catalytic ozonation, photocatalysis, and photo ozonation, respectively. ESR spectra show that much more ·OH radicals are generated in SCOP than the sum in photocatalysis and catalytic ozonation processes, indicating the synergism between two processes and explaining the high mineralization efficiency in SCOP. Finally, eight intermediates were identified by LC-MS analysis and the initial degradation pathway of tetracycline in SCOP was proposed. Excellent treatment efficiency, high ozonation utilization (>93%) and low energy consumption (14.9 KJ/mg TOC) suggest that SCOP is a promising choice for antibiotics-containing wastewater treatment.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2013
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IF 5.825
Qizhou Dai,Jiayu Wang,Jie Yu,Jun Chen,Jianmeng Chen
A magnetic core/shell CeO 2 nanometer catalyst particle of Fe 3 O 4 @SiO 2 @CeO 2 for ozonation was prepared and the catalytic activity was evaluated by the degradation of acetylsalicylic acid (ASA). The characterizations of the magnetic nanoparticles, such as TEM, XRD and EDX, showed that Fe 3 O 4 @SiO 2 @CeO 2 had a ternary structure with a Fe 3 O 4 magnetic core, a silica membrane mid-layer and CeO 2 outer layer. The catalysts of Fe 3 O 4 @SiO 2 @CeO 2 showed an obviously high efficiency in catalytic ozonation on the degradation of ASA, and thus could also enhance the TOC removal. The ASA removal with Fe 3 O 4 @SiO 2 @CeO 2 catalyst at 60 min could reach 81.0%, while 67.3% with Fe 3 O 4 @SiO 2 , 66.1% with Fe 3 O 4 and only 64.1% with ozonation alone. Fe 3 O 4 @SiO 2 @CeO 2 catalysts could also enhance the ozone utilization during the reaction. The effect of radical scavengers showed that the high removal efficiency of catalytic ozonation over Fe 3 O 4 @SiO 2 @CeO 2 may be mainly attributed to surface reactions. According to stability and recyclability test of the Fe 3 O 4 @SiO 2 @CeO 2 catalysts, the results showed that the catalysts would be helpful in the separation and magnetic recyclability. In addition, based on the intermediates detected by GC/MS, a possible degradation pathway of ASA was proposed.
研究领域:
环境科学
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催化材料
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DOI
高影响因子
Environmental Progress & Sustainable Energy
·
2016
·Vol. 35
·期 4
·975-981
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IF 1.631
Rongrong Miao,Minli Wang,Junjun Shen,Ping Ning,Junjie Gu,Qingqing Guan,Qiuling Chen,Xinsheng Chai
The sub/supercritical water oxidation (SCWO) of wastewater with high concentrations of pollutants from tall oil rosin production base was studied under the temperature range of 320°C–420°C and the pressure range of 11–25 MPa. The results showed that after pretreatment with Ca(OH) 2 for ions removal, around 385 mg/L remained which inhibited the oxidation activity by reducing the concentration of hydroxyl radicals (•OH). Since the wastewater compounds were mainly cyclic organic materials, higher O 2 contents (stoichiometric ratio over 2.5) and temperatures (over 380°C) are favorable for TOC removal. With O 2 SR = 2.5 and T = 420°C, the TOC removal reached almost 100% (99.89%) in 30 min. A global kinetic model for TOC removal during SCWO treatment was built during the research. The kinetic data acquired through the model were fitted to a power-law function, and the data correlated well with the experimental data. © 2016 American Institute of Chemical Engineers Environ Prog, 35: 975–981, 2016
研究领域:
环境工程
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化学工程
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DOI
高影响因子
CHEMOSPHERE
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2021
·
IF 7.086
Yong Chen,Junfeng Zhao,Lu Hu,Jing Tian,Yong Liu
Most metal-organic frameworks (MOFs) are synthesized from carboxylate and metal precursors by hydrothermal process, which will consume a large amount of solvent and carboxylate. To address this issue, a new strategy for Cu-based MOFs was developed, in which the Cu-based MOFs was obtained by using abundant natural polymer (tannic acid) as one of the precursors and using high-energy ball milling to achieve a self-assembly of tannic acid and copper sulfate. Based on this strategy, a novel Cu-based MOFs derivative (Cu x O@C composite) was synthesized by high-temperature sintering of Cu-based MOFs and used for sulfamerazine (SMR) removal via O 2 activation. The BET specific surface area and average pore size of Cu x O@C composite were 110.34 m 2 g −1 and 21.06 nm, respectively, which made Cu x O@C composite had the maximum adsorption capacity ( Q max ) for SMR of 104.65 mg g −1 and favored the subsequent degradation of SMR. The results from XRD and XPS indicated that Cu x O@C composite contained a lot of Cu 0 and Cu 2 O with the sizes of 76.6 nm and 9.8 nm, respectively, which led to its high performance of O 2 activation. The removal efficiency of SMR and 90.2% TOC achieved 100% and 90.2%, respectively in the Cu x O@C/air system at initial pH of 4.0, air flow rate of 100 mL min −1 , Cu x O@C dosage of 1 g L −1 and reaction time of 30 min. Reactive species, including H 2 O 2 , OH and O 2 - radicals were detected in the Cu x O@C/air system, and OH and O 2 - were mainly responsible for the degradation of SMR.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Bei Wu,Zhiqiang Jiang,Weidong Lei,Jie Sun,Zhi Chen
In a conventional electro-Fenton system with a single cathode, it is difficult to attain both high H 2 O 2 generation by oxygen reduction reaction (ORR) and efficient iron reduction reaction (FRR). For this study, a flow-through dual-system electro-Fenton (FT-DEF) reactor was designed to overcome this shortcoming and promote mass transfer to effectively remove dimethyl phthalate (DMP) from water. By comparing the ORR and FRR performances of four different commercial carbon electrodes, the graphite felt with the highest amount of H 2 O 2 generation was selected as the cathode of the ORR system, and the activated carbon fiber with the best Fe (III) reduction effect was selected as another cathode of the FRR system. The ORR system and FRR system operate simultaneously to form the DEF system. The FT-DEF system displayed many advantages compared with the conventional electro-Fenton (CI-ORR), presenting an improved efficiency and low energy consumption in phthalates removal. Under optimal reaction conditions, the FT-DEF system is capable to degrade 100% DMP in 20 min, which is 25% higher than the CI-ORR, while the reaction rate constant (0.271 min −1 ) is 16 times that of CI-ORR system (0.017min −1 ). In addition, the TOC removal of FT-DEF achieving 72.3% within 2 h with energy consumption of 2.35 kW h·m −3 is much better than CI-ORR that only achieves 18.3% TOC removal within 2 h with energy consumption of 8.13 kW h·m −3 . Furthermore, control parameters and mechanism of FT-DEF were investigated in detail. The main intermediate products of DMP were analyzed by UPLC-ESI-HRMS, and the possible degradation path of DMP was speculated. In addition, application of FT-DEF in three types of natural water demonstrated its universal applicability of the system.
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