International Journal of Environmental Research and Public Health
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2019
·Vol. 16
·期 10
·1781
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IF 2.468
Yixin Lu,Wenlai Xu,Haisong Nie,Ying Zhang,Na Deng,Jianqiang Zhang
The degradation effect, degradation mechanism, oxidation kinetics, and degradation products of Atrazine (ATZ) by Ultrasound/Peroxymonosulfate (US/PMS) in phosphate buffer (PB) under different conditions were studied. It turned out that the degradation rate of US/PMS to ATZ was 45.85% when the temperature of the reaction system, concentration of PMS, concentration of ATZ, ultrasonic intensity, and reaction time were 20 °C, 200 μmol/L, 1.25 μmol/L, 0.88 W/mL, and 60 min, respectively. Mechanism analysis showed that PB alone had no degradation effect on ATZ while PMS alone had extremely weak degradation effect on ATZ. HO• and SO4−• coexist in the US/PMS system, and the degradation of ATZ at pH7 is dominated by free radical degradation. Inorganic anion experiments revealed that Cl−, HCO3−, and NO3−showed inhibitory effects on the degradation of ATZ by US/PMS, with Cl−contributing the strongest inhibitory effect while NO3−showed the weakest suppression effect. According to the kinetic analysis, the degradation kinetics of ATZ by US/PMS was in line with the quasi-first-order reaction kinetics. ETA with concentration of 1 mmol/L reduced the degradation rate of ATZ by US/PMS to 10.91%. Product analysis indicated that the degradation of ATZ by US/PMS was mainly achieved by dealkylation, dichlorination, and hydroxylation, but the triazine ring was not degraded. A total of 10 kinds of ATZ degradation intermediates were found in this experiment.Keywords:ultrasound;peroxymonosulfate;free radicals;ATZ;degradation mechanism
研究领域:
环境科学
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化学
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DOI
PubMed
高影响因子
MOLECULES
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2022
·Vol. 27
·期 14
·4524
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IF 4.927
Tingting Wu,Huan Peng,Xiaowei Liu,Ruijin Wu
Carbamazepine (CBZ), as a typical pharmaceutical and personal care product (PPCP), cannot be efficiently removed by the conventional drinking water and wastewater treatment process. In this work, the CoS2/Fe2+/PMS process was applied for efficient elimination of CBZ. The CBZ removal efficiency of CoS2/Fe2+/PMS was 2.5 times and 23 times higher than that of CoS2/PMS and Fe2+/PMS, respectively. The intensity of DMPO-HO• and DMPO-SO4•−followed the order of Fe2+/PMS < CoS2/PMS < CoS2/Fe2+/PMS, also suggesting the CoS2/Fe2+/PMS process has the highest oxidation activity. The effects of reaction conditions (e.g., CoS2dosage, Fe2+concentration, PMS concentration, initial CBZ concentration, pH, temperature) and water quality parameters (e.g.,SO42−,NO3−,H2PO4−,Cl−,NH4+, humic acid) on the degradation of CBZ were also studied. Response surface methodology analysis was carried out to obtain the best conditions for the removal of CBZ, which are: Fe2+= 70 µmol/L, PMS = 240 µmol/L, CoS2= 0.59 g/L. The sustainability test demonstrated that the repeated use of CoS2for 8 successive cycles resulted in little function decrease (<10%). These findings suggest that CoS2/Fe2+/PMS may be a promising method for advanced treatment of tailwater from sewage treatment plant.Keywords:cobalt disulfide;persulfate;carbamazepine;advanced oxidation process
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
CARBOHYDRATE POLYMERS
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2022
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IF 10.723
Yuhang Wu,Yuwen Li,Tao Zhao,Xue Wang,Vera I. Isaeva,Leoid M. Kustov,Juming Yao,Junkuo Gao
Metal-organic frameworks (MOFs) and their derived powder catalysts are prone to agglomerate and difficult to recycle in water, thus resulting in their low utilization and secondary pollution in water treatment. Herein, a composite aerogel (CoFe0.8@NCNT@CA) loaded with bimetallic MOF-derived carbon nanotubes on cellulose aerogel was developed for activating peroxymonosulfate (PMS) to degrade tetracycline (TC). The CoFe0.8@NCNT@CA/PMS system exhibits an excellent TC removal rate (97.1 % TC removal within 20 min). The outstanding performance of the composite catalyst is closely related to the synergistic effect of bimetallic catalytic sites, graphitic N structure, and porous network. Interestingly, carbon nanotubes and cellulose in the composite catalyst form a semi-coated porous structure, which can effectively enhance the adhesion of carbon nanotubes and expose abundant active sites while ensuring mass transfer. This study provides a strategy for synthesizing novel composite aerogel with an excellent structure and physicochemical properties for water treatment.
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
Journal of Water Process Engineering
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2024
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IF 6.3
Miaomiao Ye,Wen Jin,Xingyuan Wang,Yueqian Yan,Xiaohong Zhou,Ziyi Luo,Tuqiao Zhang,Xiaowei Liu
Activation of peroxymonosulfate by heterogeneous catalyst is an efficient process for organic pollutants removal. However, it is difficult for solid-liquid separation of the heterogeneous catalysts in slurry-like batch reaction. In this work, CoS 2 particles were deposited onto an air-laid cloth (denoted as CoS 2 -ALC) and were used as a catalyst for activation of peroxymonosulfate (PMS). Unlike traditional slurry-like batch reaction forms, a shallow continuous flow reactor was designed for the installation of a CoS 2 -ALC, thereby improving the activation efficiency of persulfate and rapid solid-liquid separation. The degradation kinetics constant for carbamazepine (CBZ) by the CoS 2 -ALC/PMS process was 0.0748 min −1 , which is 374, 150, 150 times higher than that the CoS 2 -ALC adsorption process, PMS/ALC oxidation process and PMS alone process, respectively. The significantly enhanced degradation efficiency was due to the S in CoS 2 promoting the cycling of Co 2+ /Co 3+ , thereby enhancing the generation of free radical. Parameters such as CoS 2 deposition amount, PMS concentration, water flow rate, water flow height, water flow direction, solution pH, humic acid and anions that affecting the degradation efficiencies were studied. In addition, the degradation by-products of CBZ as well as their toxicity were detected, and a possible degradation pathway were proposed. Finally, expanded outdoor experiments and cycling experiment demonstrated that the CoS 2 -ALC/PMS process is potentially useful in practical settings of wastewater treatment .
研究领域:
环境科学
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废水处理
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DOI
高影响因子
Applied Sciences-Basel
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2023
·Vol. 13
·期 5
·3182
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IF 2.7
Chuning Zhang,Huaqiang Chu,Qian Ma,Yanyan Chen,Jianwei Fan
It is important to further enhance the performance of green and efficient non-homogeneous catalysts for advanced oxidation process of Peroxymonosulfate (PMS-AOP) for green treatment of industrial wastewater. In this paper, nitrogen–sulfur co-doped MOFs-derived carbon material (CoSN@C) was prepared by one-pot synthesis followed by carbonization, and its morphological structure was characterized by XRD and SEM. After pyrolysis, the CoSN@C still maintained the dodecahedral morphology and structure of ZIF-67. The synergistic effects of S and N significantly elevated the activation of PMS. The results show that the CoSN@C + PMS system can effectively activate PMS to degrade Rhodamine B (RhB), with a rate constant (1.85 min−1) four times higher than that of the CoN@C + PMS system (0.44 min−1). The optimal catalytic process parameters of material dosage, PMS concentration, temperature, pH, and other parameters were also investigated for the activation of PMS to remove Rhodamine B. The cyclic experiment shows that the CoSN@C has excellent recyclability and the degradation rate of RhB still reached 88.9% after four cycles. Radical capture experiments and EPR tests showed that the CoSN@C + PMS system generated a large amount of SO4·−and ·OH radicals adsorbed on the catalyst surface and a certain amount of singlet oxygen, and the free radical pathway and non-radical pathway worked together to degrade RhB efficiently and rapidly. While non-radical pathway with singlet oxygen as main reactive oxygen species played a key role in the CoN@C + PMS system. This work provides a new idea for the rational design of non-homogeneous catalysts for PMS-AOP system.Keywords:advanced oxidation process;peroxymonosulfate (PMS);non-homogeneous catalyst;MOFs
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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DOI
高影响因子
CHEMOSPHERE
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2024
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IF 8.1
Yuexinxi Wang,Shizong Wang,Yong Liu,Jianlong Wang
Heterogeneous activation of peroxomonosulfate (PMS) has been extensively studied for the degradation of antibiotics. The cobalt ferrite spinel exhibits good activity in the PMS activation, but suffers from the disadvantage of low PMS utilization efficiency. Herein, the nanocomposites including FeS, CoS 2 , CoFe 2 O 4 and Fe 2 O 3 were synthesized by hydrothermal method and used for the first time to activate PMS for the removal of sulfamethoxazole (SMX). The nanocomposites showed superior catalytic activity in which the SMX could be completely removed at 40 min, 0.1 g L −1 nanocomposites and 0.4 mM PMS with the first order kinetic constant of 0.2739 min −1 . The PMS utilization efficiency was increased by 29.4% compared to CoFe 2 O 4 . Both radicals and non-radicals contributed to the SMX degradation in which high-valent metal oxo dominated. The mechanism analysis indicated that sulfur modification, on one hand, enhanced the adsorption of nanocomposites for PMS, and promoted the redox cycles of Fe 2+ /Fe 3+ and Co 2+ /Co 3+ on the other hand. This study provides new way to enhance the catalytic activity and PMS utilization efficiency of spinel cobalt ferrite.
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
Journal of the Taiwan Institute of Chemical Engineers
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2017
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IF 4.217
Chaoqun Tan,Yujie Dong,Lei Shi,Qin Chen,Shengwei Yang,Xiaoyu Liu,Jinfeng Ling,Xuefeng He,Dafang Fu
The degradation of Orange II (Org II) by ferrous activated peroxymonosulfate (PMS) was inspected. The maximum degradation efficiency of 62.3% in 90 min occurred at 0.286 mM [PMS] 0 , corresponding to 1:1 molar ratio of Fe 2+ : PMS. Results show that poor recovery of Fe 2+ accounts for poor degradation in the slow stage. The species of reactive radicals were determined through indirect way by quenching agents, as well as directly by in situ EPR spin trapping tests. Results indicated that hydroxyl radicals instead of sulfate radicals were responsible for Org II degradation. The removal of Org II degradation would increase to 93.3% in 90 min as reaction temperature increased to 60 °C. The activation energy for PMS and Fe 2+ /PMS alone was calculated to be 77.2 kJ/mol and 34.7 kJ/mol, respectively. The removal efficiency of total organic carbon (TOC) was 11.0% and 43.8% when [Fe 2+ ] 0 :[PMS] 0 :[Org II] 0 was 5:5:1 and 34:34:1, respectively. The main degradation products of Org II in system were supposed to be heterocyclic compounds containing a five-atom ring. Results demonstrated that Fe 2+ /PMS technology is promising technology for water pollution.
研究领域:
环境科学
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化学工程
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高影响因子
Journal of Water Process Engineering
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2020
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IF 3.465
Zhuang Lin,Wenlei Qin,Lei Sun,Xiangjuan Yuan,Dongsheng Xia
The degradation of Bisphenol A (BPA) in the vacuum ultraviolet/ ultraviolet/ peroxymonosulfate (VUV/UV/PMS) process based on a mini-fluidic VUV/UV photoreaction system has been comprehensively investigated focusing on the degradation performances and kinetics in this study. With 20 min reaction at pH 7.0 in VUV/UV/PMS process, the removal efficiency and the apparent degradation rate constant ( k app ) of BPA were > 95.2 % and 0.145 min −1 (R 2 = 0.9935). In addition, the impacts of operational parameters and co-existing constituents on BPA degradation are systematically evaluated. Importantly, the effective degradation of BPA (> 96.1 % at least) achieved at the test pH conditions (5–11) after 30 min reaction and achieved the highest BPA removal rate at pH = 11 (0.243 min −1 , R 2 = 0.9952). The electron paramagnetic resonance and radical scavenger experiments confirmed that both hydroxyl radical ( OH) and sulfate radical (SO 4 − ) are the predominant reactive radicals in VUV/UV/PMS process. The second-order reaction rate constants of BPA with OH and SO 4 − under different pH conditions were determined to be 0.74–1.86 × 10 10 M −1 s −1 and 2.92–5.01 × 10 9 M −1 s −1 via the competition kinetics. Meanwhile, the relative contribution rate of OH decreased from 97.2 %–33.1 % with the increasement of pH from 5.0 to 11.0, while the relative contribution rate of SO 4 − rose from 1.7 % to 48.9 %. The present study demonstrated that the VUV/UV/PMS process, as a new advanced oxidation process, has potential applications for micropollutants removal in water.
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
Desalination and Water Treatment
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2024
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IF 1
Shuohua Zhou,Weiming Xiang,Qiang Zhong,Shaogui Yang,Gancheng Zuo,Zhe Xu,Qiuyi Ji,Jijie Kong,Chenmin Xu,Bing Yang,Dunyu Sun,Yinhao Dai,Yazi Liu,Huan He,Shiyin Li
Sulphate radical (SO 4 · - ) -based advanced oxidation process (SR-AOP) is a promising sewage treatment technology. Reduced graphene oxide (rGO) supported Co 3 O 4 composites were synthesized by a hydrothermal method for the degradation of iohexol (IOH) in the rGO/Co 3 O 4 /peroxymonosulfate (PMS) system. Experimental results show that rGO/Co 3 O 4 possessed much better PMS activated ability than pure GO or Co 3 O 4 , which is ascribed to the summation of rGO and Co 3 O 4 . The efficiency of rGO/Co 3 O 4 composite, single GO and Co 3 O 4 nanocrystals for the degradation of IOH were 98.7%, 15.8% and 79.8% at 15 min, and their corresponding reaction rate constants ( k app ) were 0.21 min −1 , 0.0077 min −1 and 0.080 min −1 , respectively. The results of active species capture experiment and electron paramagnetic resonance (EPR) experiment, showed that singlet oxygen is the main active species, which is non-radical degradation. rGO is conducive to the electron conduction of Co 3 O 4 , thus improving the efficiency of PMS activation. The system is simple and efficient, which is an effective technology to remove IOH.
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
Engineering
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2024
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IF 10.1
Jinjing Huang,Xia Liu,Kaixing Fu,Shengyun Yang,Shiqing Zhou,Jinming Luo
The valorization of Chinese medicine residues (CMRs) into high-value-added products, such as microcrystalline cellulose (MCC), has garnered significant interest in the current post-pandemic era, particularly in regions where Chinese medicine (CM) is widely utilized (i.e., Southeast Asia). In this study, we propose a facile and economical protocol for selectively extracting MCC from CMRs via one-step direct peroxymonosulfate (PMS) oxidation without the need for intricate steps. Importantly, our proposed protocol has been verified to be versatile and can be applied to various solid waste sources rich in cellulose, with an average extraction rate of 75%. Analysis using the Fukui index revealed that the β-O-4 bond, the aromatic ring in lignin, specific O sites in hemicellulose, and the amorphous region of cellulose are more susceptible to electrophilic attack by PMS than to reactions involving HO • , SO 4 •− , or 1 O 2 . Leveraging this distinct mechanism, the extracted MCC demonstrated ultrahigh purity (∼95%) and crystallinity (∼85.36%). Overall, our work involves transforming solid waste into high-value products through the provision of a technical solution, with the potential for onsite application. This represents a significant advancement to the valorization of CMRs, particularly in providing theoretical guidance for accelerating the recycling of waste materials.
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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废物管理
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药学
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产品关联
DOI
高影响因子
CHEMOSPHERE
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2021
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IF 7.086
Jingyi Fu,Li Feng,Yongze Liu,Liqiu Zhang,Shuo Li
Electrochemical activation of peroxymonosulfate (PMS) at carbon cloth anode (E (Carbon cloth Anode)/PMS system) was investigated for sulfamethoxazole (SMX) degradation. The results indicated that PMS could be activated at carbon cloth anode during electrolysis, resulting in the improvement of SMX degradation. The degradation efficiency of SMX was facilitated with the higher PMS concentration and current density, respectively. The degradation rate constant of SMX increased with the rising pH from 3.6 to 6.0, and reached the highest value at pH 6.0, and then decreased with further increasing pH to 8.0. The presence of chloride ion (Cl − , 5–100 mM) significantly enhanced SMX degradation, while addition of humic acid (HA, 1–5 mgC L −1 ) inhibited SMX degradation. Addition of carbonate (HCO 3 − , 5–20 mM) had a negligible impact on SMX degradation. Small amounts of phosphate (PO 4 3− , 0–5 mM) could promote degradation, while a large amount of PO 4 3− (10–20 mM) inhibited the degradation. Moreover, the quenching experiments demonstrated that sulfate radical (SO 4 · − ), hydroxyl radical (·OH) and singlet oxygen ( 1 O 2 ) contributed to SMX degradation in E (Carbon cloth Anode)/PMS system. The degradation intermediates of SMX were identified by LC-MS/MS and the degradation pathways were deduced to be hydroxylation, the cleavage of S–N bond, and oxidation of aniline group. Moreover, the micronucleus test of Vicia faba root tips indicated that the E (Carbon Cloth Anode)/PMS system could reduce the genetic toxicity of SMX contaminated water to some extent.
研究领域:
环境化学
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电化学
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水处理
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毒理学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING RESEARCH & DESIGN
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2023
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IF 3.9
Hongyu Liu,Xin Wen,Jun Zhang,Huan Zhang,Junfu Wei
Catalytic oxidation of contaminants by peroxomonosulfate (PMS) was coupled with membrane filtration to realize high-performance removal of dyes. CoFe 2 O 4 (CFO) was enwrapped and cross linked in calcium alginate (CaAlg) to form CFO−CaAlg composite membrane. The introduction of CFO could not only activate PMS, but also enhanced the stability, hydrophilic property and crosslinking degree of the composite membrane. The final removal rate was enhanced greatly benefiting from the synergistic effect of filtration and catalytic degradation. The removal rate increased from 75% (filtration) to 98% by coupling with catalytic degradation. More importantly, purified water could be obtained immediately instead of waiting for purifying the whole feed solution due to the superiority of cross flow filtration . Radicals quenching and electron spin resonance (ESR) analysis experiment confirm that SO 4 · − contributed 25% and 1 O 2 contributed 75% in catalytic degradation. The composite membrane was effective for different type of dyes and could be reused only being backwashed by purified water because the catalyst CoFe 2 O 4 could recover from Co 3+ to Co 2+ by itself during the process. This study opens a new path of rapid water purification and immediate drinking water supply.
研究领域:
环境科学
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化学工程
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高影响因子
危险品化学品经营许可证（带存储）