COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Xi Quan,Jun Zhang,Linlin Yin,Yu Tian
In this study, the activation of peroxymonosulfate (PMS) and selective degradation of nonsteroidal anti-inflammatory drugs were investigated using hydrophobically modified Fe 3+ @Cu-MOF. The Fe 3+ @Cu-MOF-CTAB/PMS system demonstrated high-efficiency, achieving near-complete degradation of diclofenac within 120 min. The degradation rate constants for diclofenac, ibuprofen, and naproxen were 0.0048, 0.00103, and 0.00046 min −1 , respectively, positively correlated with their hydrophobicity. Longer hydrophobic surfactant chains in Fe 3+ @Cu-MOFs lead to greater initial adsorption of diclofenac, enhancing degradation efficiency upon the introduction of PMS. The Fe 3+ @Cu-MOF-CTAB/PMS system removes over 80 % of diclofenac in various water matrices, showing optimal efficiency in acidic environments but reduced effectiveness with competing anions. Post-degradation changes in the oxidation states of copper and iron in the MOF structure indicated a synergistic redox mechanism essential for PMS activation. The hydroxylation and C-N bond cleavage in diclofenac were key degradation pathways. This study highlights the potential of hydrophobically modified Fe 3+ @Cu-MOFs in water treatment, providing insights into the interplay between material design, hydrophobic interactions, and catalytic performance.
研究领域:
环境科学
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催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Ziyang Chu,Zhengyan Han,Haibo Liu,Tianhu Chen,Xuehua Zou,Hanlin Wang,Fuwei Sun,Hao Wang,Dong Chen
The simultaneous removal of heavy metal complexes (HMCs) and heavy metal ions presents a significant challenge in treating wastewater. To address this, we propose a Calcite/Peroxymonosulfate (Calcite/PMS) system aimed at simultaneously decomplexing Cu-EDTA and removing Cu ions . Calcite/PMS system could achieve 99.5 % Cu-EDTA decomplexation and 61.9 % Cu ions removal within 60 min under initial conditions of Cu-EDTA (10 mg/L), Calcite (3 g/L), and PMS (2 mM). Singlet oxygen ( 1 O 2 ) emerged as the predominant reactive species responsible for Cu-EDTA decomplexation, which selectively targeted the N-C bonds in the Cu-EDTA structure to produce intermediates with lower biotoxicity than EDTA. Interestingly, solid phase Cu(III) (≡Cu(III)) promoted the generation of superoxide radicals (O 2 •− ) with a contribution of up to 72.8 %. Subsequently, nascent ≡Cu(III) and O 2 •− accelerated the degradation of intermediates. Besides, coexisting organic substances inhibited Cu-EDTA decomplexation, whereas inorganic ions had a weak impact. After five cycles of use, the Calcite/PMS system retained 99.3 % efficiency in decomplexing Cu-EDTA. This investigation provides valuable insights into using calcite to remove HMCs and enhances our comprehension of the decomplexation intermediates accelerating HMCs degradation.
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
Journal of Water Process Engineering
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2025
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IF 6.7
Qianyi Wang,Wan Yu,Wenjun Xu,Zhen Li,Xiren Xia,Yin Xu
Doping strategies are widely employed to enhance the catalytic activity of perovskites for peroxymonosulfate (PMS) activation in removing organic pollutants in water. However, limited research has explored the performance enhancement and underlying mechanism associated with trace doping, which is particularly important for saving dopant metals and cost, and also lower the risk of metal ion loss. In this study, we investigated the profound effects of trace copper doping in LaMnO 3 on PMS activation for contaminant removal. Compared to pristine LaMnO 3 , the catalytic oxidation performance was significantly enhanced by trace copper doping (1.3 wt% Cu), achieving over 91.0 % removal of acid orange 7 (AO7) within 45 min using the LaMn 0.95 Cu 0.05 O 3 (LMC5)/PMS system. Comprehensive characterizations revealed that copper incorporation primarily fortified the redox ability and electron transfer efficiency of LaMnO 3 , thereby improving its catalytic efficacy. Furthermore, unlike previous studies reporting on radical oxidation mechanisms, the surface PMS* complexes with Mn(III) serving as the active sites were identified as the predominant reactive species responsible for pollutant degradation. The intermediates of pollutant degradation were identified and their toxicity was also assessed by ECOSAR program. The system's practical feasibility was further underscored by treating diverse contaminants and evaluating the interference of coexisting anions in water. Briefly, this study provides valuable insights into enhancing the catalytic activity of perovskites for PMS activation in water treatment.
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
APPLIED CATALYSIS A-GENERAL
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2020
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IF 5.006
Wenyan Wang,Yunlan Xu,Dengjie Zhong,Nianbing Zhong
Removal of complexation metal from plating effluents is always a problem. In this work, a core-shell structure zero-valent iron@nitrogen/graphite carbon nitride doped carbon (ZVI@C-N/g-C 3 N 4 ) composite was prepared and used to activate peroxymonsulfate (PMS) to treat complexation nickel simulated wastewater. Compared with ZVI, ZVI@C-N/g-C 3 N 4 significantly enhanced the efficiency and repeatability of PMS activation. For 45 min treatment, the removal efficiency of 50 ppm Ni-EDTA and Ni-citrate simulated wastewater reached 95.8 % and 100 %, respectively. The excellent performance of ZVI@C-N/g-C 3 N 4 is attributed to that the amino groups of nitrogen in C-N/g-C 3 N 4 shell can regulate the transmission rate of electrons released from ZVI core by adjusting the transmission rate of H + , so as to improve the electron utilization efficiency of PMS activation.
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 ELECTROANALYTICAL CHEMISTRY
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2022
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IF 4.598
Yaxin Zhang,Zhuang Chen,Yimei Zhang,Wenwen Gu,Wendy Huang,Jiangshan Xi,Ting Cao,Yingjie Yu,Mingwang Yang,Luoyilang Ke
In this system, a highly-exposed TiO 2 photoanode was prepared as an effectively photoelectrocatalyst peroxymonosulfate (PMS) activator. Especially, we realize the highly-exposed TiO 2 grown on negatively charged MXene nanosheet which could provide dual active sites for stimulating PMS. The catalysts were characterized by XRD, XPS, SEM, UV–vis, Raman, TEM, and BET. The specific surface area for highly-exposed TiO 2 (S-400) is 10 times than Bulk catalyst (B-400), which is displayed in the BET result. The experimental results show that high exposure catalyst has excellent photoelectric activation performance. The degradation efficiency of the PEC + PMS system was 2.94 times higher than the EC + PMS and 2.76 times higher than the PC + PMS process. Compare with free PMS (1.36˚A), PMS adsorbed at the photoanode interface has a high bond angle (2.85˚A) easily to decompose into strong oxidizing SO 4 − . The electrochemical characterization results demonstrated that the highly-exposed TiO 2 had a higher separation rate of photogenerated carriers. From quenching experiments, the holes (h + ) contributed 80 % to BPA degradation in PEC + PMS system, the contribution order of other active radicals was O 2 − >SO 4 − > OH. It will help improving the control of the optimal free radical ratio. The probable mechanism and pathway of BPA degradation were suggested e − reacts with PMS and other substances to generate radicals. The research offers a new strategy for the effective activation about PMS to oxidation of the refractory organics. Besides, the results provide useful theoretical guidance for the development of new high-activity materials.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Haoran Song,Shiting Pan,Yuwei Wang,Yang Cai,Wei Zhang,Yongming Shen,Changping Li
There exists an obvious contradiction between Cu(III) generation and Cu(I) contribution in reductants enhanced Cu(II)/peroxymonosulfate (PMS) process because the involved electron transfer pathways were always ignored in previous studies. This study investigated the MXene-mediated electron transfer mechanism in Cu(II)/PMS for the first time. The introduction of MXene significantly promoted atrazine degradation under acidic condition because the in-situ generation of Cu(I) was an excellent activator for PMS. Under alkaline condition, although addition of MXene generated a large amount of Cu(I), the degradation of atrazine was inhibited due to that the conversion of Cu(I) to Cu(III) was interrupted. The strong metal-support interaction (SMSI) altered the reactive intermediate species from Cu(III) (two-electron transfer) to hydroxyl radical (HO • ) and sulfate radical (SO 4 •- ) (one-electron transfer) under alkaline condition. This work proposed a novel MXene-mediated electron transfer mechanism and improved the understanding of Cu(III)/Cu(I) transformation pathway.
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
RSC Advances
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2023
·Vol. 13
·期 22
·15063-15076
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IF 3.9
Song Wang,Yonggang Zhang
Advanced oxidation processes are frequently applied to a variety of refractory organic wastewater, but rarely is electro-Fenton combined with activated persulfate technology applied to the removal of refractory pollutants. In this work, the electro-Fenton process was combined with zero-valent iron (ZVI) activated peroxymonosulfate (PMS), two advanced oxidation processes based on different radicals, to form the ZVI-E-Fenton-PMS process to treat wastewater, whose main advantages are the generation of more reactive oxygen species and the reduction of oxidant cost to achieve rapid removal of pollutants. This process can not only produce H2O2 and activate PMS at the cathode, but also reduce Fe(III) to realize the sustainable Fe(III)/Fe(II) redox cycle. The main reactive oxygen species in the ZVI-E-Fenton-PMS process were found to be ˙OH, SO4˙− and 1O2 by radical scavenging experiments and electron paramagnetic resonance (EPR), and the relative contributions of the three reactive oxygen species for the degradation of MB were estimated to 30.77%, 39.62% and 15.38%, respectively. Then, by calculating the ratio of the relative contributions of each component to the removal of pollutants at different PMS doses, it was found that the synergistic effect of the process was better when the proportion of ˙OH in the oxidation of reactive oxygen species (ROS) was higher and the proportion of non-ROS oxidation increased year-on-year. This study provides a new perspective on the combination of different advanced oxidation processes and reveals the advantages and potential of this process for application.
研究领域:
环境工程
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水处理
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化学工程
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高级氧化技术
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DOI
PubMed
高影响因子
Water
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2023
·Vol. 15
·期 15
·2856
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IF 3.4
Jing Wang,Huanyu Zhou,Li Ma,Quanfeng Wang,Da Sun,Libo Jin,Guoming Zeng,Jujiao Zhao
Peroxymonosulfate (PMS) activation has gained increasing attention for its water remediation. In this work, carbon nanotube-supported FeCo2O4nanoparticles (FeCo2O4/CNT) were prepared and showed tremendous potential as a catalyst for PMS activation. The synergistic effect between FeCo2O4and CNT in FeCo2O4/CNT promotes its better catalytic performance than individual CNT or FeCo2O4. The synthesized FeCo2O4/CNT could reach 100% phenol removal with akvalue of 0.30 min−1within 15 min ([PMS] = 0.3 g L−1, [FeCo2O4/CNT] = 0.3 g L−1). FeCo2O4/CNT can adapt well to a wide pH range (4–9) and a complex water component (with inorganic ions or organic matter). Moreover, the catalytic mechanism investigation suggested that both radical and non-radical pathways are accountable for the efficient removal of phenol.Keywords:peroxymonosulfate;FeCo2O4/CNT;phenol removal
研究领域:
环境科学
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催化化学
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DOI
高影响因子
ENVIRONMENTAL TECHNOLOGY
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2023
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IF 2.8
Zhendong Wang,Zhexin Zhu,Gangqiang Wang,Xiaoji Ma,Wangyang Lu
Iron (II) phthalocyanine (FePc) is loaded on the surface of the tourmaline (TM) by the reflow method to obtain FePc/TM. This research effectively prevents the π-π stacking of FePc, increased the effective utilization rate of PMS activation under solar light, and further improved the catalytic performance of the catalytic system. The catalytic oxidation efficiency of FePc/TM on carbamazepine (CBZ) and sulfadiazine (SD) can reach 99% under solar light for 15 and 5 min, the total organic carbon (TOC) removal rate can reach 58% and 69% under solar light for 120 min. After 6 cycles, the CBZ removal rate remained above 95%. In addition, the FePc/TM catalytic system has an excellent removal rate for other pharmaceuticals. The results of spin-trapped electron paramagnetic resonance and classical quenching experiments show that FePc/TM can effectively activate PMS to generate active species under solar light, including superoxide radical (•O2−), singlet oxygen (1O2), hydroxyl radicals(•OH), and sulphate radicals (SO4•−). The intermediates of CBZ were identified by Ultra-high performance liquid chromatography and high resolution mass spectrometry, and the degradation pathway was proposed. As the reaction progresses, all CBZ and intermediates are reduced and converted into small acids, or mineralized to H2O, CO2. This work provides an alternative method for the design of efficient activation of PMS activation catalysts under solar light to eliminate residual pharmaceuticals in actual water bodies.
研究领域:
环境科学
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催化化学
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污染控制
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产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2021
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IF 5.909
Linhai Yang,Xuechang Ren,Yujie Zhang,Zuoyan Chen
This article is an in-depth study of the basis of Cu + -decorated triazine-based g-C 3 N 4 (Cu + /g-C 3 N 4 ) nanosheet-activated H 2 O 2 . In this study, peroxymonosulfate (PMS) was activated by Cu + /g-C 3 N 4 under sunlight and used to treat simulated wastewater RhB. The properties of g-C 3 N 4 and Cu + /g-C 3 N 4 were characterized by UV–Vis DRS and PL . The results indicated that the introduction of Cu + in g-C 3 N 4 can enhance the separation of photogenerated electron-hole pairs. The Cu + /g-C 3 N 4 (1:4) samples exhibited the best PMS activation performance under sunlight when 0.5 g/L catalyst dose and 0.5 mmol/L PMS concentration were used, and the removal rate of RhB reached 95.7% in 30 min. Moreover, better catalytic activity of the system can be achieved in the initial pH range of 2.0–10.0. The investigation results of the catalytic mechanisms showed that the prepared Cu + /g-C 3 N 4 catalyst constructs a dual reaction center of Cu + /Cu 2+ cycling and e CB − / h VB + transfer for efficient PMS activation. The degradation of pollutants benefits from the participation of a variety of free radicals, which are generated by sunlight-assisted heterogeneous activation of PMS. This study has resulted in substantial progress in activating multiple oxidants with a single heterogeneous catalyst and provides a feasible way to treat refractory wastewater using Cu + /g-C 3 N 4 with PMS under sunlight.
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
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Mengjie Pu,Daqi Ye,Jinquan Wan,Bentuo Xu,Wei Sun,Wei Li
A novel peroxymonosulfate (PMS) catalyst, zinc-based metal–organic framework electrospinning (ES) nanofibers membrane (short for ZIF-65/PAN) was firstly fabricated and used for the degradation of aqueous ciprofloxacin (CIP). Physicochemical properties, catalytic performance, stability, reusability, and the regeneration of ZIF-65/PAN was observed and conducted. Influence of various parameters including ZIF-65 loading content, reaction temperature, initial pH, and competitive organic molecules on CIP degradation was investigated. Reactive active species and degradation intermediates that involved in ZIF-65/PAN/PMS/CIP process were identified. Corresponding reaction mechanisms were speculated. The results indicate that the easy-separation ZIF-65/PAN nanofibers exhibit high efficiency for PMS activation, 89.2 % of CIP was degraded within 60 min, with up to 87.5 % of PMS utilization efficiency. ZIF-65/PAN was renewable through simple layer-by-layer self-assembly, thus shows good prospect in future applications. 26.4 % of surface Zn 2+ of ZIF-65/PAN exists in the form of + III oxidation state after activation, indicating the role of zinc catalytic site. Through activation, oxidative active species SO 4 ·− , ·OH, and 1 O 2 was generated, CIP was thus degraded through mainly-three pathways. This study provides novel ideas for the application of MOF-based membrane on PMS based advanced oxidation processes.
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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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yonglei Xing,Huimin Ma,Jian Yi,Xiaoyong Jin,Yage Peng,Gang Ni
Antibiotic pollutants such as levofloxacin (LVF) pose serious threats to ecosystems and human health due to their persistence in aquatic environments, making their efficient removal a great challenge. In this study, a BiFeO 3 /BiVO 4 heterojunction photoanode was rationally designed for the photoelectrocatalytic (PEC) degradation of levofloxacin (LVF) in the presence of peroxymonosulfate (PMS). Under visible light irradiation and a 0.6 V bias, the BiFeO 3 /BiVO 4 photoanode coupled with PMS achieved 78 % LVF degradation, markedly surpassing bare BiVO 4 (≈44 %), with excellent mineralization and stability, retaining > 72 % efficiency after four cycles. Radical quenching experiments revealed the synergistic roles of SO 4 •− , ‧O 2 − , ‧ OH , and h + . To clarify the PMS activation pathway, a dual-chamber H-type reactor with a proton exchange membrane was employed, confirming that PMS activation originated from photogenerated electrons at the photoanode, while the cathode contribution was negligible. Photoelectrochemical analyses (OCP, DPV, EIS, i–t) further demonstrated the adsorption–activation–electron capture behavior of PMS. These findings highlight BiFeO 3 /BiVO 4 as a promising photoanode for PMS-assisted PEC degradation of antibiotics, offering an effective strategy for water purification.
研究领域:
环境科学
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材料化学
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光催化
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水处理技术
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产品关联
DOI
高影响因子
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