Catalysts
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2022
·Vol. 12
·期 10
·1100
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IF 4.501
Jingxin Tan,Guoqiang Wei,Zhen Wang,Hui Su,Lingtao Liu,Chunhu Li,Junjie Bian
Zn1−xCdxS catalysts with Zeolitic Imidazolate Framework-8 (ZIF-8) as the precursor were successfully prepared by ion exchange method, and the ability and electrochemical properties of a series of ZIF-8, ZnS and Zn1−xCdxS catalysts in photocatalytic degradation of 2-CP and TC were investigated. Doping of Cd ions was able to modulate the ZnS band gap width and improve the utilization of visible light by the photocatalyst. The nanocage catalysts with hollow structure of Zn1−xCdxS have better photocatalytic response. The removal of photocatalytic pollutants was up to 90% under optimal conditions. Using a Peroxymonosulfate (PMS)-assisted system to improve the degradation efficiency of 2-chlorophenol and tetracycline hydrochloride under visible light, we present a possible mechanism of Zn1−xCdxS as a photocatalyst for degradation in persistent pollutants and in PMS-assisted photocatalysis. Four active species, O2−, h+, -OH, and SO4•−, can be generated to degrade 2-chlorophenol and tetracycline hydrochloride under PMS-assisted activation. Zn1−xCdxS nanocage with high activity and stability provides a feasible approach to catalytically remove persistent pollutants from aqueous solutions under visible light conditions.Keywords:nanocage photocatalyst;Zn1−xCdxS;2-CP;TC;PMS;degradation
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
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Ziwei Gao,Tao Zhang,Md. Nahid Pervez,Guojuan Qu,Wei Jin,Yaping Zhao
Materials combing catalytic and adsorption dual active sites are very important for arsenite (As(III)) due to its high mobility in water. Therefore, in this study, a bifunctional walnut-like Co-doped La(OH) 3 composites (Co-La) with independent catalytic sites and post-formed adsorption sites were synthesized via a simple hydrothermal method. Nearly 100% As(III) removal can be achieved in Co-La and peroxymonosulfate interaction systems (Co-La/PMS) within 10 min at the molar ratio of PMS to As(III) of 1.2. The results indicate that the combined Co-La adsorption system demonstrated superior performance compared to the Co-La adsorption alone. Precisely, the maximum removal capacity of the system was measured at 243.90 mg·g −1 , and the pseudo-first-order kinetic rate constant ( k 1 ) was determined to be 1.0771 min −1 . These values were significantly greater than those observed for Co-La adsorption alone. Notably, the kinetic rate constant was 239 times faster, and the removal capacity was 4.6 times higher in the combined system. The fast kinetics of As(III) elimination can be elucidated by the production of reactive oxygen species (ROS) such as S O 4 · - , •OH, O 2 · - and 1 O 2 , which expedite the conversion of As(III) into arsenate (As(V) in this particular system. Meanwhile, the increase in adsorption capacity is ascribed to the fact that PMS can drive La(OH) 3 of Co-La to transform into transition states La 2 SO 4 (OH) 4 , thus generating a new exchangeable adsorption site for As(V). A fixed membrane reactor assembled with Co-La was utilized to achieve a near-complete removal of As(III) within 3 min. The Co-La/PMS systems demonstrate exceptional effectiveness in eliminating arsenic from water across diverse real-water metrics, offering a unique perspective and technological progress in purifying water contaminated with arsenic.
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
·
IF 11.357
Xiao-Chi Feng,Zi-Jie Xiao,Hong-Tao Shi,Bai-Qin Zhou,Yong-Mei Wang,Hui-Zhong Chi,Xiao-Hang Kou,Nan-Qi Ren
Current research has widely applied heteroatom doping for the promotion of catalyst activity in peroxymonosulfate (PMS) systems; however, the relationship between heteroatom doping and stimulated activation mechanism transformation is not fully understood. Herein, we introduce nitrogen and sulfur doping into a Co@rGO material for PMS activation to degrade tetracycline (TC) and systematically investigate how heteroatom doping transformed the activation mechanism of the original Co@rGO/PMS system. N was homogeneously inserted into the reduced graphene oxide (rGO) matrix of Co@rGO, inducing a significant increase in the degradation efficiency without affecting the activation mechanism transformation. Additionally, S doping converted Co3O4 to Co4S3 in Co@rGO and transformed the cooperative oxidation pathway into a single non-radical pathway with stronger intensity, which led to a higher stability against environmental interferences. Notably, based on density functional theory (DFT) calculations, we demonstrated that Co4S3 had a higher energy barrier for PMS adsorption and cleavage than Co3O4, and therefore, the radical pathway was not easily stimulated by Co4S3. Overall, this study not only illustrated the improvement due to the heteroatom doping of Co@rGO for TC degradation in a PMS system but also bridged the knowledge gap between the catalyst structure and degradation performance through activation mechanism transformation drawn from theoretical and experimental analyses.
研究领域:
环境科学
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材料科学
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理论化学
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DOI
PubMed
高影响因子
Nanomaterials
·
2023
·Vol. 14
·期 1
·74
·
IF 5.3
Xin Zhong,Meihuan Ji,Wenxin Wu,Caicai Lu,Wenping Liu,Fubin Jiang
In this work, the heterojunctions of CuInS2embedded in the g-C3N4materials (xCuInS2/g-C3N4, abbreviated as xCIS/GCN) was successfully prepared for peroxymonosulfate (PMS) activation under visible light. The catalysts are characterized by different techniques, such as XRD, FTIR, SEM, TEM, and UV-vis. The unique heterojunction composites can suppress the recombination of photogenerated pairs. The catalytic results showed that the 3CIS/GCN exhibited excellent catalytic levofloxacin (LVF) degradation efficiency, while more than 98.9% of LVF was removed in 60 min over a wide pH range. SO4•−, O2•−, OH•, and1O2were verified as the main reactive species for LVF degradation via the quenching experiments and electron paramagnetic resonance technology (EPR). The synergetic effect of xCIS/GCN, PMS, and visible light irradiation was discussed. The possible LVF degradation pathway was proposed through byproducts analysis (LC-MS). Moreover, the 3CIS/GCN/vis-PMS system has very low metal leaching. Owing to xCIS/GCN having good properties for PMS activation, it has potential applications for LVF or other hazardous pollutants degradation.Keywords:peroxymonosulfate;visible-light-assisted PMS activation;antibiotics
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
ACS ES&T Water
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2025
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IF 4.3
Yin Li,Jiahui Hu,Lin Lin,Bing Li,Xiao-yan Li
Transition metal-activated peroxymonosulfate (PMS) processes are extensively studied for pollutant degradation, with phenyl methyl sulfoxide (PMSO) commonly used as a probe for detecting high-valent metal species. However, recent studies have attributed PMSO oxidation to reactive oxygen species generated from PMS self-decomposition, raising concerns about the probe’s specificity. This study systematically evaluated PMSO oxidation under varying pH conditions to reassess its reliability. The results showed that the PMSO degradation and methyl phenyl sulfone (PMSO2) formation increased significantly with rising pH. This pH-dependency, intrinsic to the PMS/PMSO system, indicates potential interference from PMS itself. Multiple analytical approaches indicate that 1O2 and O2•- generated from PMS self-decomposition make negligible contributions, whereas PMS itself is the primary oxidant converting PMSO to PMSO2. Kinetic studies revealed that SO52– primarily drives PMSO oxidation via nucleophilic attack, with a rate constant of 10.44 M–1s–1, far exceeding that of HSO5– (0.037 M–1 s–1). Theoretical calculations further confirmed that PMSO is relatively resistant to nucleophilic attack by SO52–, making it a comparatively reliable sulfoxide probe in acidic and neutral PMS systems. These findings highlight the limitation of PMSO as a high-valent metal probe under alkaline conditions and offer guidance for probe selection in future studies.
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高影响因子
APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Guanwei Peng,Yanyu Xie,Ying Wang,Qi Yu,Youyi Huang,Shuwu Liu,Limin Lu
Peroxymonosulfate (PMS)-assisted photocatalytic processes are economical and green strategies for the treatment of pesticide pollution. However, its degradation efficiency is severely hindered by the sluggish kinetics of active centers regeneration and low charge-transfer. Herein, S-scheme Bi 2 Fe 4 O 9 /BiOBr heterogeneous material was designed to activate PMS for thiabendazole (TBZ) degradation. Bi 2 Fe 4 O 9 and BiOBr have similar structural unit of [Bi 2 O 2 ] 2+ to share the Bi-O bonds, which is favorable to form asymmetric interface and enhance the polarization. Based on these unique characteristics between Bi 2 Fe 4 O 9 and BiOBr, a robust internal electric field in the S-scheme heterojunction is built, which could provide driving force to boost the electron-transfer process and encourage the sustainable regeneration of Fe 2+ . After optimizing the proportion of Bi 2 Fe 4 O 9 on the composite, it was found that 50 wt% Bi 2 Fe 4 O 9 /BiOBr (BFB-50) exhibits the best TBZ removal efficiency after 30 min visible light irradiation, which is 2.25 and 12 folds compared to Bi 2 Fe 4 O 9 and BiOBr, respectively. Furthermore, electron paramagnetic resonance (EPR) and radical trapping experiments indicate that 1 O 2 and SO 4 •- involving oxidation mechanism impart maximum contribution towards TBZ degradation. The possible pathways of TBZ degradation are reasonably proposed by the HPLC-MS and the toxicity evolution of TBZ is appraised using the ECOSAR software. This study provides an insight into the fabrication of S-scheme heterojunction for environment remediation through the photocatalysis/sulfate-mediated advanced oxidation process.
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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2023
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IF 8.6
Bingxuan Ji,Yang Li,Zhenghua Zhang
Membrane distillation (MD) provides a potential method to supply large volumes of good quality potable water from surface water resources, avoiding the risk of long-term water shortages. However, the high abundance of dissolved natural organic matter (DOM) in surface water induces severe membrane fouling, which reduces productivity and increases energy consumption. Therefore, for the first time, electrochemically activated peroxymonosulfate (PMS) treatment was applied prior to the direct contact (DC)-MD process with the aim of reducing the deposition of organics and inorganics on the membrane and reducing membrane fouling. Results showed that supplying PMS continuously at a rate of 0.10 mM/min, eliminated 30.4% of dissolved organic carbon (DOC). Furthermore, fluorescence parallel factor (PARAFAC) analysis showed that >60% of two fluorescent substances were removed after 60 min of the electrochemically activated PMS pretreatment at a current density of 5 mA/cm 2 . Electrochemical activation of PMS generated •OH directly, facilitating the removal and degradation of DOM. In terms of the DCMD performance, almost no normalized flux decline was observed for the DCMS process after 0.01 mM/min pre-oxidation, while 44.8% flux decay occurred in the standalone DCMD treating raw surface water. Compared with continuous dosing, the use of a one-time dosing mode achieved a better outcome, as more small organic molecules generated in continuous dosing mode are not conducive to membrane fouling control. Therefore, electrochemically activated PMS could be an effective tool to mitigate membrane fouling in MD processes, although the characteristics of membrane and feed should be considered.
研究领域:
环境工程
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水处理
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膜技术
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化工工程
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DOI
高影响因子
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Zhongsen Yan,Binbin Li,Guohui Liu,Zhenyu Lu,Haiqing Chang,Juxiang Jin,Wenxin Dai,Yao Qu,Fangshu Qu
Humic acid (HA), a widely prevalent natural organic matter in aquatic environments, poses serious health risks due to its potential to form carcinogenic by-products during water treatment. While the photo-Fenton process can be employed for HA degradation, its effectiveness is often hindered by the poor catalytic performance of conventional catalysts. In this study, Co 3 O 4 was modified with nitrogen-doped carbon quantum dots (NCDs) and immobilized on a PVDF membrane. Compared with Co 3 O 4 /PVDF, Co 3 O 4 /NCDs/PVDF system achieved 85.1 % HA removal and 66 % mineralization within 60 min through photocatalytic peroxymonosulfate (PMS) activation as well as showed excellent stability in cycle experiments. The incorporation of NCDs enhanced the synergistic effect between light and PMS, improved light absorption due to the narrowed bandgap of Co 3 O 4 /NCDs/PVDF, and played a significant role in generating the primary reactive species, 1 O 2 . Additionally, Co 3 O 4 /NCDs/PVDF effectively controlled Co ions leaching. Finally, the degradation intermediates were identified, and the degradation pathways were proposed. The photo-Fenton degradation of HA preferentially broke unsaturated bonds and degraded aromatic ring compounds. The Co 3 O 4 /NCDs/PVDF photo-Fenton catalytic system serves as an effective approach for boosting the efficiency of photo-Fenton degradation.
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
JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Xiaoyu Fu,Jingfeng Gao,Qian Wang,Hao Chen,Ying Liu,Liqin Zeng,Yukun Yuan,Hongxin Xu
The existence of antibiotic resistant bacteria (ARB) and antibiotic resistance genes (ARGs) has been a global public environment and health issue. Due to the different cell structures, gram-positive/negative ARB exhibit various inactivation mechanisms in water disinfection. In this study, a gram-negative ARB Escherichia coli DH5α ( E. coli DH5α) was used as a horizontal gene transfer (HGT) donor, while a gram-positive ARB Bacillus as a recipient. To develop an efficient and engineering applicable method in water disinfection, ARB and ARGs removal efficiency of Fe(VI) coupled peroxydisulfate (PDS) or peroxymonosulfate (PMS) was compared, wherein hydroxylamine (HA) was added as a reducing agent. The results indicated that Fe(VI)/PMS/HA showed higher disinfection efficiency than Fe(VI)/PDS/HA. When the concentration of each Fe(VI), PMS, HA was 0.48 mM, 5.15 log E. coli DH5α and 3.57 log Bacillus lost cultivability, while the proportion of recovered cells was 0.0017 % and 0.0566 %, respectively, and HGT was blocked. Intracellular tetA was reduced by 2.49 log. Fe(IV) and/or Fe(V) were proved to be the decisive reactive species. Due to the superiority of low cost as well as high efficiency and practicality, Fe(VI)/PMS/HA has significant application potential in ARB, ARGs removal and HGT inhibition, offering a new insight for wastewater treatment.
研究领域:
环境科学
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微生物学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Xiaoxiao Zhang,Zhonglin Chen,Jing Kang,Shengxin Zhao,Binyuan Wang,Pengwei Yan,Fengxia Deng,Jimin Shen,Wei Chu
In this study, kinetics, influencing factors and potential mechanisms involved in the degradation of chloral hydrate (CH) by UV/peroxymonosulfate (PMS) process were demonstrated. The degradation rate of CH could reach 89.6% by UV 254 /PMS process, significantly exceeding UV 300 /PMS (0.7%), UV 350 /PMS (6.3%), UV 254 direct photolysis (9.0%) and PMS alone (0.0%) processes. CH degradation in UV 254 /PMS system followed pseudo first-order degradation kinetics with an apparent rate constant of 0.186 min −1 , which was suppressed by Cl − and HCO 3 − . The optimal pH for CH degradation was around 5.0. Direct mineralization accounted for the CH degradation in UV/PMS system. Interestingly, the addition of PMS at the neutral condition before UV irradiation transferred CH into trichloroacetic acid (TCAA). The transformation efficiency of CH into TCAA at 10 min was enhanced from 2.17%–40.38% with the elevation of initial pH from 7.0–8.0. The subsequent exposure of UV lamps ceased the transformation of CH into TCAA and facilitated the direct mineralization of CH, but it did not work in the refractory TCAA degradation. Finally, it was revealed that HO predominantly participated CH degradation in UV/PMS process, while O 2 − was responsible for the transformation of CH into TCAA by addition of PMS before UV irradiation.
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
Environmental Technology & Innovation
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2022
·
IF 7.758
Waseem Hayat,Ze-hua Liu,Yi-ping Wan,Yongqing Zhang
This study concentrated on degradation of fenuron (FEN) from aqueous solutions by manganese dioxide (MnO 2 )-peroxymonosulfate (PMS) system. The performance of commercial (c)MnO 2 , beta (b)MnO 2 and alpha (a)MnO 2 in combination with PMS was investigated. The degradation efficiency of applied systems followed the order: aMnO 2 -PMS system > bMnO 2 -PMS system > cMnO 2 -PMS system. The 38.0% degradation of 20.0 mg/L was achieved by aMnO 2 -PMS system after 180 min at initial pH 7.0 using 0.6 g/L aMnO 2 and 2.0 mmol/L PMS. The degradation by aMnO 2 -PMS system was affected by initial PMS and FEN concentrations, aMnO 2 dosage, pH and temperature. The degradation decreased with increasing pH from 3.0 to 11.0 and increased with increasing temperature from 25.0 ± 0 . 5 ∘ C to 40.0 ± 0 . 5 ∘ C. The radical quenching analysis showed that sulfate radical (SO 4 ⋅− ) was primarily responsible for degradation. The comparison of degradation efficiency of aMnO 2 -PMS system with degradation efficiencies of pyrite (PyR)-PMS system as well as zero-valent iron (ZVI)-PMS system revealed that activated PMS is not favorable for efficient degradation of fenuron from aqueous solutions.
研究领域:
环境科学
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水处理
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yizhou Wu,Wenqi Zhou,Liang Zhou,Su-Il In,Juying Lei,Lingzhi Wang,Jinlong Zhang,Yongdi Liu
The utilization of near-infrared (NIR) light with strong photothermal effect in photo-Fenton or Fenton-like systems for the degradation of organic pollutants is always ignored. In this study, we have synthesized a novel photothermal Fenton-like catalyst (Co 3 O 4 /PDA) to activate peroxymonosulfate (PMS) for the degradation of antibiotics. The Co 3 O 4 in the nanocomposite acts as a PMS activator, while unexpectedly, PDA was found to accelerate the redox cycle of Co 2+ /Co 3+ . Both Co 3 O 4 and PDA are black-colored photothermal materials with excellent NIR absorption properties. During the degradation process, the light-to-heat conversion ability of Co 3 O 4 and PDA enables a higher temperature, which innovatively boosts the rate of PMS catalytic activation. Mechanistic studies revealed that the increased temperature effectively promotes the heterogeneous catalytic PMS activation by Co 3 O 4 /PDA. As a result, the Co 3 O 4 /PDA + PMS + NIR system exhibits greatly enhanced degradation performance. Furthermore, this degradation system demonstrates strong tolerance to different operation conditions, and the catalyst exhibits good stability in cycling tests. These results demonstrate the favorable application prospects of this photothermal Fenton-like system in environmental water remediation. The findings also contribute valuable insights towards the development of efficient strategies for the photothermal activation of PMS.
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
危险品化学品经营许可证（带存储）