ENVIRONMENTAL RESEARCH
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2023
·
IF 8.3
Wen Qin,Jianshan Peng,Jingru Yang,Yang Song,Jun Ma
In this study, the relative residual UV absorbance (UV 254 ) and/or electron donating capacity (EDC) was investigated as a surrogate parameter to evaluate the abatement of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes. In the Fe(II)/PMS process, due to the generation of SO 4 •- and •OH at acidic pH, UV 254 and EDC abatement was greater at pH 5. In the Mn(II)/NTA/PMS process, UV 254 abatement was greater at pH 7 and 9, while EDC abatement was greater at pH 5 and 7. This was attributed to the fact that MnO 2 was formed at alkaline pH to remove UV 254 by coagulation, and manganese intermediates (Mn(V)) were formed at acidic pH to remove EDC via electron transfer . Due to the strong oxidation capacity of SO 4 •- , •OH and Mn(V), the abatement of micropollutants increased with increasing dosages of oxidant in different waters in both processes. In the Fe(II)/PMS and Mn(II)/NTA/PMS processes, except for nitrobenzene (∼23% and 40%, respectively), the removal of other micropollutants was greater than 70% when the oxidant dosages were greater in different waters. The linear relationship between the relative residual UV 254 , EDC and the removal of micropollutants was established in different waters, showing a one-phase or two-phase linear relationship. The differences of the slopes for one-phase linear correlation in the Fe(II)/PMS process (micropollutant-UV 254 : 0.36–2.89, micropollutant-EDC: 0.26–1.75) were less than that in the Mn(II)/NTA/PMS process (micropollutant-UV 254 : 0.40–13.16, micropollutant-EDC: 0.51–8.39). Overall, these results suggest that the relative residual UV 254 and EDC could truly reflect the removal of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes.
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
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
Yongjun Huang,Zixiang He,Xiaobin Liao,Yusheng Cheng,Huan Qi
Carcinogenic N , N -Dimethylnitrosamine (NDMA) has been reported to generate significantly during ozonation of fuel additive unsymmetrical dimethylhydrazine (UDMH), the combined ozone/Peroxy-Monosulfate (O 3 /PMS) technology was tried for reducing its formation in this study. The influence of PMS dosages, ozone concentrations, pH, Br - and humic acid (HA) on NDMA formation from UDMH were investigated. In addition, the reduction mechanisms were explored by intermediates identification and Gaussian calculation. The results demonstrated that O 3 /PMS technology was effective on NDMA reduction, reaching an efficiency of 81% with 80 μM PMS. Higher NDMA reduction rates were achieved by O 3 /PMS with increasing pH within the scope of research (from 5 to 9), achieving a maximum of 69.9% at pH 9. The presence of bromide ion facilitated NDMA generation during ozonation, but the reduction efficiency by O 3 /PMS slightly improved from 66.3% to 70.6%. The presence of HA reduced NDMA formation in O 3 /PMS system. The contribution of SO 4 •− on NDMA reduction accounted for ~64%, which was higher than that of •OH (41.4%); however, its promotion role on conversing UDMH to NDMA was lower than O 3 . Therefore, the technology could reduce NDMA formation effectively. In addition, the results of Gaussian calculation manifested that the N atom in -NH 2 group of UDMH was easily attacked not only by •OH but also by O 3 , so it is the key path that determines final NDMA formation. This study would provide reference for reducing NDMA formation during ozonation of UDMH-containing water matrixes.
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
CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Ying Fang,Baoyu Qian,Ying Yang,Yang Song,Zhaoguang Yang,Haipu Li
Purification of high-arsenic (>10 µg/L) groundwater is of significance for drinking water safety all around the world. Considering the dominant presence of arsenite (As(III)) in groundwater and ineffective adsorption of As(III) by traditional adsorbents, the magnetic Zn/Co bimetallic MOFs (Zn/Co MOFs) which contain both catalytic and adsorption sites were prepared, and coupled with peroxymonosulfate (PMS) to realize the efficient simultaneous oxidation of As(III) and adsorption of evolved As(V). Considering the vital roles of oxidation and adsorption, the molar ratio of Zn and Co precursors was tuned ranging from 1: 1 to 9: 1 during Zn/Co MOFs synthesis to balance the catalysis and adsorption processes in the heterogeneous PMS system for As(III) immobilization. It was found that Zn/Co MOFs with Zn and Co molar ratio of 5: 1 possessing moderate catalytic performance and best adsorption capacity outperformed removal performance for As(III). The presence of PMS significantly promoted the elimination of both As(III) (the initial adsorption rate increased from 31.19 to 358.96 µg/g/min) and As(V) (the initial adsorption rate increased from 354.12 to 497.85 µg/g/min), which not only oxidized As(III) into As(V) by reactive species generated from PMS activation but also provided additional adsorption sites through enlarging pore size and changing chemical environment. Furthermore, Zn/Co MOFs coupled with the PMS system exhibited outstanding reusability and effectiveness for remediation of real high-arsenic groundwater.
研究领域:
环境科学
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材料科学
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高影响因子
Processes
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2023
·Vol. 11
·期 3
·903
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IF 3.5
Yajie Wang,Xin Dong,Chengfeng Liu,Peng Cheng,Gilles Mailhot
The decolorization of azo dye Orange II using a UVA-Fe3+-PMS-oxalate system was studied. A series of experiments was performed to investigate the effects of several variables, including the pH, PMS dosage, Fe3+concentration, oxalate concentration, and coexisting anions. The results revealed that a lower pH facilitated the decolorization, and relatively high decolorization efficiency (97.5%) could be achieved within 5 min at pH 3.0. The electron paramagnetic resonance (ESR) and radical quenching experiments revealed that SO4•−played a crucial role in the decolorization of Orange II (85.8%),•OH was of secondary importance (9%), and1O2made a small contribution to the decolorization (5.2%). Furthermore, the formation of•OH in the experimental system strongly depended on HO2•/O2•−. These reactive oxidants were able to directly attack the azo bond of the luminescent group in Orange II and initiate the decolorization process. The efficient UVA-Fe3+-PMS-oxalate system showed great application potential in the treatment of wastewater contaminated by azo dyes.Keywords:PMS activation;Orange II;decolorization;UVA irradiation;Fe3+-oxalate complexes
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 HAZARDOUS MATERIALS
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2023
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IF 13.6
Shenjun Wang,Xiaonan Tan,Yuhao Wu,Jun Zhang,Zhiyuan Tian,Jiahai Ma
Rapid isolation of microplastics is the prerequisite for correct and in-depth understanding of their environmental impacts and human health threats. And Fenton’s reagent (Fe/H 2 O 2 system, FHS) has been proven to be a viable way to isolate microplastics from wastewater, but it is limited because of harsh reaction conditions, long reaction time and low efficiency. Herein, it's proven that the Fenton-like system, which is using Cobalt (II) salts to decompose potassium peroxymonosulfate (Co/PMS system, CPS) with generation of 1 O 2 , can offer shorter time (within 30 min) in complex sample isolation. The experimental results showed that the isolation time of micro/nanoplastics from pollutants with CPS in only 30 min, while it was at least more than 5 h with FHS. Via a serious of experiments of comparison and characterization between FHS and CPS, whether from the point of view of reaction time or isolation effect , CPS is superior to FHS. On this basis, we validate the applicability of this system (CPS) in different reaction conditions (concentration, pH), different sizes (from microns to nanometers) and types of plastic (PS, PA, PE, PP, PVC). In addition, the CPS can also preserve the integrity of the plastic itself and reduce the impact on the quality of samples evidenced by a variety of characterization of physicochemical structure like UV–vis, TEM, AFM , FTIR and XPS. CPS is proved to be faster, higher, stronger for enhancing the isolation of micro/nanoplastics from complex matrix. In a word, this study provides a promising solution for the efficient isolation of microplastics from wastewater without causing additional harm to the plastics.
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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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Yu-qiong Gao,Yan-yan Rao,Han Ning,Ju-xiang Chen,Qian Zeng,Fu-xiang Tian,Nai-yun Gao
The degradation of diclofenac (DCF), a commonly used nonsteroidal anti-inflammatory drug, by Fe 2+ /chlorine and Fe 2+ /PMS processes was comparatively investigated. The influencing factors of pH, Fe 2+ and oxidant dosage on DCF degradation efficiency were evaluated and optimized. Typically, with an initial solution pH of 5, an Fe 2+ dosage of 70 μM, and a chlorine or PMS dosage of 70 μM, the degradation efficiency of DCF using the Fe 2+ /chlorine and Fe 2+ /PMS processes reached 94.2% and 79.7%, respectively, within 10 min. Quenching tests indicated the coexistence of •OH and RCS in the Fe 2+ /chlorine system, and both SO 4 ●– and •OH were identified in the Fe 2+ /PMS system. In addition, Fe(IV) was also identified to participate in DCF degradation in two systems based on the oxidation of PMSO to PMSO 2 . The degradation products and pathways of DCF were elucidated by LC/TOF/MS analysis and DFT calculations. It was assumed that the degradation pathway of DCF involves hydroxylation, dechlorination, decarboxylation, cleavage of the C-N bond, and chlorine substitution. In addition, trichloromethane (TCM), dichloroacetaldehyde (DCAL), dichloroacetonitrile (DCAN) and trichloronitromethane (TCNM) were also detected in the Fe 2+ /chlorine process, and these chlorinated DBPs initially increased and then decreased with prolonged reaction time, indicating that Fe 2+ /chlorine is capable of controlling DBPs formation. Finally, the acute and chronic toxicity of DCF and its degradation products were evaluated by the ECOSAR program.
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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高影响因子
CATALYSIS LETTERS
·
2025
·Vol. 155
·期 4
·1-19
·
IF 2.4
Cheng Liu,Zhu Zhexin,Wang Gangqiang,Du Shiting
Since Peroxymonosulfate (PMS) is readily available and can produce sulfate radicals with a stronger oxidation capacity, the Fenton-like system Fe 2+ /PMS has gradually replaced Fe 2+ /H 2 O 2 system in organic pollutants degradation. However, the Fe 3+ /PMS system has almost no degradation effects, with the conversion of Fe 2+ to Fe 3+ being the rate-limiting step in the Fe 3+ /PMS system. In this paper, graphite-like phase carbon nitride (g-C 3 N 4 ) was employed to activate PMS using trace amounts of Fe 3+ for the treatment of water pollution under sunlight, and the Fe 3+ /g-C 3 N 4 /PMS system demonstrated the ability to rapidly degrade a wide range of difficult-to-degrade organic pollutants. The Fe 3+ /g-C 3 N 4 /PMS system was able to completely degrade carbamazepine (CBZ) within 30 min under sunlight. The fundings indicated that this system effectively improved the stringent limitations typically associated with Fenton process regarding the feed ratio of metal ions to oxidants, and could efficiently degrade CBZ across a broad pH range. In addition, the Fe 3+ concentration of 6.17 × 10 −6 M was used in the experiments to avoid the generation of large amounts of “iron sludge”. The trap burst experiments, DMSO oxidation experiments and electron paramagnetic resonance spectroscopy experiments indicated that O 2 · − and 1 O 2 exerted the major effectiveness in the photocatalytic degradation reaction of CBZ, and SO 4 · − and · OH jointly promoted the CBZ degradation. Graphical
研究领域:
环境科学
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化学
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Lulu Long,Changwei Bai,Xinyu Zhou,Shirong Zhang,Yanzong Zhang,Chao Chen,Jingsong He,Chun Song,Gang Yang
This study proposed a novel strategy to improve the activation efficiency of PMS by enhancing the utilization of side reactions. Electrocatalysis and PMS activation were coupled in the anode chamber. The electrons were extracted from the catalyst through the electroanode, and the excess low valence elements in the system were converted into high valence elements. Without restricting the activation of PMS, the activation efficiency of PMS was more effectively and comprehensively improved by enhancing the utilization of side reactions. An efficient electrocatalytic anode/Mn 2 O 3 /rGO/peroxymonosulfate (ECA/Mn 2 O 3 /rGO/PMS) system was established with Mn 2 O 3 /rGO as the anode. In this system, the anode current improved the catalyst utilization, which directly converts the excess rGO-C = O, Mn(II) and Mn(III) into rGO-C + -O, Mn(III) and Mn(IV), thereby increasing the yields of •OH, SO 4 • - , and 1 O 2 during PMS activation. Overall, this study provides a novel strategy for improving the activation efficiency of PMS, and has great potential to be widely applied in actual environment remediation.
研究领域:
环境科学
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化学工程
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电化学
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高影响因子
Nanoscale
·
2023
·Vol. 15
·期 16
·7352-7364
·
IF 6.7
Xiaojuan Bai,Wei Song,Xuan Ling,Linlong Guo,Derek Hao,Xiao Zhang
The rational design of photocatalytic nanomaterials with unique structures is critical for remediating environmental problems and thus reducing ecological risks. In this work, we employed H2 temperature-programmed reduction to modify MFe2O4 (M = Co, Cu, and Zn) photocatalysts for obtaining additional oxygen vacancies. After activation of PMS, naphthalene and phenanthrene degradation rates in the soil phase were increased by 3.24-fold and 1.39-fold, respectively, and 1.38-fold for naphthalene in the aqueous phase by H-CoFe2O4−x. The extraordinary photocatalytic activity is attributed to the oxygen vacancies on the H-CoFe2O4−x surface, which promote electron transfer and thus enhance the redox cycle from Co(III)/Fe(III) to Co(II)/Fe(II). In addition, oxygen vacancies are used as electron traps to hinder the recombination of photogenerated carriers and accelerate the generation of hydroxyl and superoxide radicals. Quenching tests showed that the addition of p-benzoquinone resulted in the greatest decrease in the degradation rate of naphthalene (inhibition of about 85.5%), demonstrating that O2˙− radicals are the main active species in the photocatalytic degradation of naphthalene. H-CoFe2O4−x showed improved degradation performance in synergy with PMS (82.0%, kapp = 0.00714 min−1) while maintaining excellent stability and reusability. Hence, this work provides a promising approach for the design of efficient photocatalysts to degrade persistent organic pollutants in soil and aqueous environments.
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
Journal of Environmental Chemical Engineering
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2025
·
IF 7.2
Zong-Bin Lv,Lei Xu,Chen Chen,Ze-Hang Chen,Ming-Lai Fu,Baoling Yuan
The outstanding performance of LiFePO4 batteries has driven their widespread adoption in electric vehicles and energy storage systems. Consequently, there has been a significant increase in their disposal rate, making the proper handling of Spent LiFePO4 batteries a matter of paramount concern. While various methods for recovering cathode materials from spent LiFePO4 batteries have been extensively researched, the application of advanced oxidation processes for this purpose remains relatively underexplored. Advanced oxidation process (AOP) based on Peroxy-monosulfate (PMS, 2KHSO5-KHSO4-K2SO4) is a widely adopted AOP primarily based on sulfate radicals (SR-AOPs). In this paper, a PMS-based advanced oxidation process is proposed to recover lithium from LiFePO4 batteries. Li+ in LiFePO4 is released into solution by Fe2+ being oxidized, with a Li+ leaching rate of as high as 99.9 %, and the released Li+ is recovered in the form of Li2CO3 after reacting with Na2CO3, and at the same time FePO4 is generated, with its olivine structure remaining unchanged. The optimal experimental conditions were 1.15 times of the theoretical amount of PMS, 10 g/L solid-liquid ratio, 25 °C reaction temperature, and 20 min leaching time. This study provides a new recovery scheme for selective extraction of Li+ from spent LiFePO4 batteries, which is characterized by a simple recovery process and high efficiency.
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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高影响因子
CHEMOSPHERE
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2022
·
IF 8.943
Dongdong Liu,Dengqian Chen,Zhengkai Hao,Yibo Tang,Lipeng Jiang,Tianqi Li,Bing Tian,Cuiping Yan,Yuan Luo,Boyin Jia
In this work, a comparative study of efficient degradation of Rhodamine B (RhB) in CoFe 2 O 4 /H 2 O 2 and CoFe 2 O 4 /PMS systems was performed. Batch experiments indicated that the RhB degradation rate of CoFe 2 O 4 /H 2 O 2 system reached 95.5% at 90 min under the condition of 0.5 g L −1 of CoFe 2 O 4 dosage, 10 mM of H 2 O 2 concentration and 3.0 of initial pH. At certain conditions of initial pH = 7.0, 0.3 g L −1 of CoFe 2 O 4 dosage, 7 mM of PMS concentration, CoFe 2 O 4 /PMS system could completely degrade RhB within 90 min. EPR and quenching experiments indicated that •OH was the main active species of CoFe 2 O 4 /H 2 O 2 system, and •OH, SO 4 • - , •O 2 − and 1 O 2 participated in RhB degradation of CoFe 2 O 4 /PMS system. The circulate of Co(II)/Co(III) and Fe(II)/Fe(III) on the CoFe 2 O 4 surface promoted the formation of free radical species in the two system. In CoFe 2 O 4 /PMS system, the formed •O 2 − and SO 5 • - realized the generation of non-free radical species ( 1 O 2 ). The LC-MS results indicated that N -de-ethylation, chromophore cleavage, opening rings and mineralization were the main steps for the RhB degradation of the two systems. After five cycles of degradation experiment, the CoFe 2 O 4 /H 2 O 2 and CoFe 2 O 4 /PMS systems still maintained the high degradation rate (85.2% and 92.4%) and low mass loss (2.7% and 3.09%). In addition, CoFe 2 O 4 /PMS system had better potential value for the actual water and multi-pollutant degradation than CoFe 2 O 4 /H 2 O 2 system. Finally, the toxicity analysis and cost assessment of the two oxidation systems were preliminarily evaluated.
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Shiqi Liu,Zichen Zhang,Fei Huang,Yongze Liu,Li Feng,Jin Jiang,Liqiu Zhang,Fei Qi,Chao Liu
N-doped carbonaceous materials are promising efficient catalysts for peroxymonosulfate (PMS) activation. In this study, the high-efficient N-doped carbon materials were prepared by direct carbonization of polyaniline (PANI) at 700 °C–1000 °C. It was optimized that the CPANI-9 (carbonized polyaniline prepared at 900 °C) exhibited excellent catalytic performance to activate PMS for phenol degradation, which was efficient over a wide pH range (pH 3.5∼9). In the CPANI-9/PMS system, the PMS adsorption/activation was identified as the key step determining the reaction rate. The quenching experiments and electron paramagnetic resonance demonstrated that the non-radical pathway was dominant in phenol degradation and singlet oxygen ( 1 O 2 ) was the main active specie. Graphitic N, pyridinic N, defects and ketonic groups (C O) were identified as catalytic sites. Interestingly, only the presence of PO 4 3− greatly decreased the phenol degradation rate and PMS decomposition. The CPANI-9/PMS system could also degrade effectively various organic pollutants , indicating that it had potential practical application.
研究领域:
环境科学
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化学工程
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材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）