JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xianni Song,Wenzhong Wang,Yu Guo
Methyl phenyl sulfoxide (PMSO), conventionally employed to probe high-valent metal-oxo species in persulfate processes, is reveals herein as a substrate-dependent mediator that selectively enhanced/inhibited degradation of various pollutants in Fe(II)/peroxymonosulfate (PMS) systems. Control experiments across transition-metal systems (Fe(II)/Co(II)/Cu(II)/Mn(II)/Fe(III)) confirmed that this phenomenon is unique to Fe(II)-based systems. The system-dependent behavior of PMSO is demonstrated to correlate with ROS generated in each system. In Fe(II)/PMS systems dominated by Fe IV O 2+ , SO 4 ·– and unidentified iron-centered species, PMSO exhibits dual functionality: as an electron shuttle, enhancing degradation of electron-rich pollutants by facilitating electron transfer and promoting the Fe(III)/Fe(II) cycle; conversely, for electron-deficient pollutants, PMSO functions as a conventional scavenger, suppressing degradation. Quantitative structure-activity relationships (QSARs) modeling establishes that PMSO enhances degradation for pollutants with the highest occupied molecular orbital (HOMO) ≥ −8.3154 eV and ionization potential (IP) ≤ 6.9711 eV; otherwise, it inhibits degradation. In Co(II)/PMS systems dominated by Coᴵᴵ-PMS* complexes, PMSO competitively consumes Coᴵᴵ-PMS* and quenches SO 4 – resulting in uniform inhibition of all pollutants. Negligible PMSO effect was observed in Cu(II)/Mn(II)/Fe(III) systems with ineffective PMS activation. This work challenges the uncritical use of PMSO as an inert probe in Fe(II) systems, highlights metal-peroxo complexes as pivotal intermediates dictating electron-transfer pathways and provides principles for designing selective advanced oxidation processes (AOPs) through mediator tuning.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Frontiers of Environmental Science & Engineering
·
2017
·Vol. 12
·期 2
·1-10
·
IF 1.716
Jiang Wenchao,Tang Ping,Lu Shuguang,Zhang Xiang,Qiu Zhaofu,Sui Qian
The performance of sodium percarbonate (SPC) activated with ferrous ion (Fe(II)) with the addition of formic acid (FA) to stimulate the degradation of carbon tetrachloride (CT) was investigated. Results showed that CTcould be entirely reduced within 15 min in the system at a variety of SPC/Fe(II)/FA/CT molar ratios in experimental level. Scavenging tests indicated that carbon dioxide radical anion (CO 2 ∙ – ) was the dominant reactive oxygen species responsible for CT degradation. CT degradation rate, to a large extent, increased with increasing dosages of chemical agents and the optimal molar ratio of SPC/Fe(II)/FA/CT was set as 60/60/60/1. The initial concentration of CT can hardly affect the CT removal, while CT degradation was favorable in the pH range of 3.0–9.0, but apparently inhibited at pH 12. Cl – and HCO
- 3
of high concentration showed negative impact on CT removal. Cl – released from CTwas detected and the results confirmed nearly complete mineralization of CT. CT degradation was proposed by reductive C-Cl bond splitting. This study demonstrated that SPC activated with Fe(II) with the addition of FA may be promising technique for CT remediation in contaminated groundwater.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Chuanfei Zhang,Wenjun Yin,Zhangjie Yu,Xin Mao,Jinlong Wang,Bin Liu,Xiaobin Tang,Langming Bai,Guibai Li,Heng Liang
DBD/Fe(II)/PAA couples radical oxidation with in situ Fe(III) coagulation. • Plasma-driven Fe cycling sustains PAA activation and reduces pH sensitivity. • Pretreatment increased normalized NF flux by 125% and lowered R ir by 76%. • Humic-like fluorescence fell by ~90%, with complete micropollutant removal. • NF reduced total DBPs by 92% and additive cytotoxicity by 90%. Nanofiltration (NF) can polish landfill leachate but is constrained by rapid fouling by humic macromolecules and colloids. Here, we developed a dielectric barrier discharge (DBD)/Fe(II)/peracetic acid (PAA) pretreatment that couples radical oxidation with in situ coagulation to simultaneously transform macromolecular foulants and mitigate NF fouling. Mechanistic analyses revealed that DBD facilitates Fe(II)/Fe(III) redox transformation during PAA activation, while Fe(II) serves as the catalytic center for PAA activation and the precursor for in-situ Fe(III) flocs. This dynamic generates a suite of reactive species in which hydroxyl radicals ( • OH) dominate oxidation, supplemented by organic radicals (CH 3 C( O )O • , CH 3 C( O )OO • ) and high-valent Fe(IV) = O. Oxidation reduced humic-like fluorescence by approximately 90% and removed 90–95% of three model micropollutants. Concurrently, Fe(III) generated during PAA activation aggregated oxidized organics and colloids into larger, less negatively charged flocs. This coupled transformation increased normalized NF flux by 125% and decreased irreversible resistance by 76% relative to untreated leachate. The process remained effective at pH 11 because PAA decomposition and plasma chemistry acidified the reaction medium. Subsequent NF removed 92% of chlorinated disinfection byproducts and reduced additive cytotoxicity by 90%. Economic assessment indicates an operating cost of 5.76 USD ton −1 and a carbon footprint of 0.59 kg CO 2 -eq m −3 . Unlike conventional treatments, the DBD/Fe(II)/PAA process enables plasma-assisted Fe(II)/Fe(III) redox regeneration, coupling enhanced PAA activation with in situ iron coagulation to transform and remove refractory foulants for NF fouling mitigation. This work demonstrates a cost-effective and mechanistically robust pretreatment strategy for improving NF-based landfill leachate treatment. Download: Download high-res image (192KB) Download: Download full-size image
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2026
·Vol. 16
·期 6
·5501-5514
·
IF 4.6
Lian Yu,Baozi Lu,Zhen Liang,Dabin Wang,Jiarui Lu,Fengyi Wei,Cunzhen Liang
The slow rate of the Fe3+/Fe2+ cycle has decreased the efficiency of photo-Fenton technology for wastewater treatment. Here, a novel GO/MIL-100(Fe)@Fe3O4 heterostructure was constructed by growing Fe3O4 nanoparticles and MIL-100(Fe) onto GO, thus accelerating the Fe3+/Fe2+ cycle and improving catalytic activity, and it was used as a heterogeneous photo-Fenton catalyst for ERY degradation. The catalyst was fully characterized by TEM, XRD, Raman spectroscopy, XPS, N2 adsorption–desorption and UV-vis DRS. The influences of initial solution pH, H2O2 concentration and catalyst dosage on ERY degradation were investigated. Under optimal conditions (initial pH of 4.03, 10.0 mM H2O2, 0.1 g L−1 catalyst), the GO/MIL-100(Fe)@Fe3O4 + H2O2 + vis system removed 97.3% of ERY (0.1 mmol L−1) within 60 min, and the pseudo-first-order rate constant was 0.0575 min−1. Furthermore, the catalyst showed favorable stability, maintaining excellent catalytic activity even after 4 cycles. A possible degradation mechanism of ERY was proposed based on the results of characterization, ERY degradation, and reactive species analysis. Fe3O4, MIL-100(Fe) and GO in the catalyst showed synergistic effects; the photo-induced electrons from MIL-100(Fe) could be immediately transferred to Fe3O4, promoting Fe3+ reduction to Fe2+ in the photo-Fenton reaction. GO in the catalyst could promote electron transfer from MIL-100(Fe) and organics to Fe3O4, significantly promoting the Fe3+/Fe2+ cycle.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Xiong Zhang,Jian Zhao,Changqi Heng,Yiyang Lei,Minyan Yu,Zhonghua Xiang,Michael Y. Hu,Jiyong Zhao,Esen Ercan Alp,Xuning Li,Yanqiang Huang
Iron-nitrogen-carbon (FeNC) catalysts are considered among the most promising alternative to Pt catalysts in acidic oxygen reduction reaction (ORR), yet the geometric and electronic structures of the true active site under reaction conditions have not been clearly elucidated. Herein, we synthesized a representative FeNC catalyst by pyrolyzing Fe3+ absorbed on ZIF-8-derived N-doped carbon at a mild temperature under the H2/Ar atmosphere, where a formation mechanism of FeN4 sites through a Zn-mediated Fe nanoparticle atomization process was proposed. The resulting FeNC-750 catalyst shows high acidic ORR activity with a half-wave potential of 0.838 V and a peak power density of 1 W cm-2 in proton-exchange membrane fuel cell (PEMFC). By using operando57Fe Mössbauer spectroscopy on FeNC-750, it was revealed that the pyrrolic N-coordinated high-spin Fe2+N4 sites, which are in situ generated from high-spin Fe3+N4 during ORR, are identified as catalytic active states. Density functional theory calculations further verified that, compared to the pyridinic N-coordinated low-spin Fe2+N4, the pyrrolic N-coordinated high-spin Fe2+ exhibits optimized adsorption energy for reaction intermediates, thereby lowering the energy barrier of the rate-determining step (RDS) and facilitating OH* desorption. This work provides both experimental and theoretical evidence of the true active site in the FeNC during acidic ORR, offering significant insights for the rational design of high-performance materials for acidic fuel cells.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Maolin Wang,Yaling Wang,Xudong Jing,Jiahui Xu,Min Li,Qing Xie,Xiyun Cai
Iron-activated persulfate (PS) systems commonly suffer from the poor Fe(III)/Fe(II) redox cycle in groundwater and soils, due to the rapid oxidation of Fe(II) by both PS-related and naturally occurring oxidative substances. Maintaining the Fe(III)/Fe(II) redox cycle is necessary to achieve the high efficiency and stability of iron-activated persulfate systems toward aromatic contaminants (e.g., PAHs) in groundwater and soils. Herein, we discover the mixtures of dithionite (DTN) and zerovalent iron (ZVI) to synergistically activate PS, and develop highly efficient, stable DTN-ZVI/PS systems for PAHs removal in groundwater and soils. DTN and intermediates sulfite/thiosulfate initiated reduction of ZVI-derived Fe(III) species in DTN-ZVI/PS systems. This reaction accelerated the Fe(III)/Fe(II) redox cycle and coated ZVI with FeS x , both favoring the generation of HO and SO 4 − . DTN-ZVI/PS exhibited Nap removal of >90% in water during 11 of 15 supplementations of Nap and/or PS, 1.4–2.4 times ZVI/PS. Similarly, 0.47–4.3 fold increments of Nap removal k obs were obtained in five chemical types of groundwater, and 1.3–2.4 fold increments of PAHs removal in soils. This study may provide a technical basis to develop new Fe-activated oxidation systems for groundwater and soil remediation .
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Zhongmin Feng,Jingwen Yang,Liangyuan Zhu,Ting Sun
Fe–based metal–organic frameworks (Fe–MOFs) have been widely used in heterogeneous Fenton-like processes. However, the catalytic performance of Fe-MOFs is limited by the relatively slow Fe (III)/Fe (II) redox cycle. For Fe-MOFs, increasing the interfacial electron transfer and reducing the electron density of Fe-MOFs are expected to accelerate the reduction of Fe (III) and improve the catalytic performance. Here, by mixing Fe/Cu metal species and introducing bromine groups, we successfully prepared bromine-functionalized bimetallic MOFs–FeCu(BDC-Br), and we used it to effectively degrade phenol in a Fenton-like process. Compared with most other catalysts, FeCu(BDC-Br) achieved a higher phenol degradation kinetic rate of 0.106 min –1 at a low dose. Effects of pH, humic acid (HA) and coexisting ions on the degradation of phenol were examined. The FeCu(BDC-Br) /H 2 O 2 system can remove phenol in the near neutral pH range of 4–6 and 0–50 mg/L HA range. Chloride ion , sulfate, or phosphate with a concentration of 100 mg/L showed an inhibitory effect on the catalytical performance of phenol degradation. This work provides insights for the preparation of Fe-MOFs Fenton-like catalyst in water/wastewater treatment.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhenglin Chen,Guangzhen Liu,Shuiping Yu,Lixia Yang,Lingyi Zheng,Zhihui Wei,Shenglian Luo
Cathode materials with high hydrogen peroxide (H 2 O 2 ) selectivity and Fe 2+ regeneration under macroneutral conditions are the essential for practical electro-Fenton processes. Herein, we develop an amorphous cobalt sulphide (CoSx(t = x)@Cu) cocatalytic electro-Fenton (EF) system capable of effectively degrading organic pollutants, such as sulfamethoxazole, at macroneutral pH conditions. Owing to the flexible electronic properties of amorphous structures and charge redistribution triggered by S defects, the optimum CoSx(t = 8)@Cu cathode successfully introduces H*/H + and promotes the in-situ evolution of H 2 O 2 . Additionally, an acidic microenvironment was constructed on the CoSx(t = 8)@Cu surface by the unreduced H*/H + , enabling a self-adjustment from alkalinity to acidity in the EF reaction without adding acid. Such self-adjustment effectually inhibits iron sludge production and promotes Fe 2+ regeneration, assuring 80% Fe 2+ cycling efficiency. More importantly, the EF system possesses outstanding stability and applicability for organic pollutant remediation regardless of water matrices. This work elucidates the intrinsic mechanism of amorphous electrocatalysts in overcoming the pH limitation of EF reactions, extending the applicability of Fenton technology.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Junhui Yang,Wenlei Wang,Jinglin Yin,Yanmei Li,Ziyang Xiang,Yi Peng,Ying Yan,Jing Wang,Hongbo Xiao
In this study, a matrix composite material of CdZnS and α-FeOOH on carbon cloth (CZS@FeOOH@CC) was prepared by a hydrothermal method , and was used for the degradation of As(III). The composite material has good photocatalytic activity of removing As(III) in the presence of oxalate. CZS@FeOOH@CC can completely degrade 10 mg/L As(III) within 10 min under visible light irradiation. The influence factors of CZS@FeOOH@CC composite material on catalytic oxidation of As(III) were also studied in the oxalate system. The photocatalytic oxidation efficiency of As(III) is affected by the oxalate concentration in the reaction system, and the atmosphere plays a major role in the degradation of As(III). Under visible light, oxalate first combines with Fe(III) on the surface of iron oxide to form Fe(III)-oxalate complex, and then the Fe(III)-oxalate composite is activated to produce·C 2 O 4 − . In the presence of oxygen, Fe(II) readily reacts with O 2 and oxidizes to Fe(III). The introduction of CdZnS promoted the separation of interfacial electron holes, and accelerated the REDOX cycle of Fe(II)/Fe(III). This study provides a feasible and simple method for accelerating the catalytic removal of heavy metals from wastewater by iron-based materials.
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 28
·17212-17221
·
IF 3.361
Haining Song,Yifei Zhou,Zexin Li,Haifeng Zhou,Fenglei Sun,Zhenlei Yuan,Peng Guo,Guangjun Zhou,Xiaoqiang Yu,Jifan Hu
Dual-function and multi-function sensors can use the same material or detection system to achieve the purpose of detection of two or more substances. Due to their high sensitivity and specificity, dual-function and multi-function sensors have potential applications in many fields. In this article, we designed a dual-function sensor to detect Sn(II) and ascorbic acid (AA) based on the inner filter effect (IFE) between NaYF4:Yb,Er@NaYF4@PAA (UCNPs@PAA) and Fe(II)–1,10-phenanthroline complex. Fe(II)–1,10-phenanthroline complex has strong absorption in most of the ultraviolet-visible light range (350 nm–600 nm), and this absorption band overlaps with the green emission peak of UCNPs@PAA at 540 nm; Fe(II)–1,10-phenanthroline complex can significantly quench the green light emission of UCNPs@PAA. When Sn(II) or AA is added to the UCNPs@PAA/Fe(III)/1,10-phenanthroline, they can reduce Fe(III) to Fe(II). Fe(II) can react with 1,10-phenanthroline to form an orange complex, thereby quenching the green light emission of UCNPs@PAA. And the quenching efficiency is related to the concentration of Sn(II) and AA; there is a linear relationship between quenching efficiency and the concentration of Sn(II) and AA, within a certain concentration range the detection limits of this dual-function sensor for Sn(II) and AA are 1.08 μM and 0.97 μM, respectively. In addition, the dual-function sensor can also detect Sn(II) and AA in tap and spring water.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Peng Zhou,Xiaowei Huo,Jing Zhang,Yang Liu,Feng Cheng,Xin Cheng,Yunqi Wang,Yongli Zhang
Hydroxylated fullerene (fullerenol) has gained increasing attention in the field of water environment remediation based on its intrinsic properties of photosensitivity and high water solubility. In this work, C 60 fullerenol was added to the Fe(III)/PMS process to enhance diethyl phthalate (DEP) degradation both with and without visible light. The DEP removal ratio was increased from 2.2% to 58.8% with the addition of fullerenol at 60 min in dark condition, and the removal of DEP was completely achieved within 50 min under visible light irradiation. Mechanism investigation shows that carboxyl and carbonyl were formed via keto-enol isomerization at acid condition, resulting in the formation of open-cage fullerenol. The open-cage fullerenol can act as complex agent and electron donor to enhance oxidizing capability of the Fe(III)/PMS process by promoting Fe(III)/Fe(II) cycles. Competitive radical capture tests by electron spin resonance (ESR) and radical quenching analysis demonstrate that hydroxyl radical and sulfate radical were primarily responsible for DEP removal, but not superoxide radical and singlet oxygen. The DEP removal in the F/Fe(III)/PMS process is more efficiency at initial pH ranging from 2.1 to 4.9. Moreover, the DEP degradation route was proposed involving the generation of various intermediary products. This study provides a novel method for the application of fullerene derivatives on environment remediation by combining with metal catalyzed advanced oxidation processes.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Donghui Han,Jinquan Wan,Yongwen Ma,Yan Wang,Mingzhi Huang,Yangmei Chen,Dongya Li,Zeyu Guan,Ying Li
Oxidative decolorization of Orange G (OG) in Fe(II)/(S,S)-ethylenediamine-N,N′-disuccinic acid (EDDS)/persulfate (PS) process was investigated. Hydroxylamine was combined to accelerate the Fe(II) recovery for improvement of PS activation. Effects of the reagents dosage, pH, and hydroxylamine adding mode were evaluated in batch experiments. All the decolorization experiments were performed at 25 °C within 180 min and with initial OG concentration ranging from 0.25 to 2.5 mM. The results indicated that EDDS decreased the Fe(II) accessibility to 11.9% at the molar ratio of EDDS/Fe(II) = 1/1 and could improve the OG decolorization by slowing down the Fe(II) depletion rate. The addition of hydroxylamine was effective in further enhancement of the oxidative ability and 98% OG decolorization was obtained rapidly with only 50.6% PS decomposition when hydroxylamine/Fe(II) = 8/5. The combination of EDDS and hydroxylamine could expand the effective pH range up to 7. The hydroxylamine adding mode also played a significant role and OG decolorization efficiency was 49.4%, 67.7% and 70.7% when adding times was 1, 3 and 5, respectively. In addition, under the condition of PS/Fe(II)/hydroxylamine = 5/10/16, OG suffered incomplete decolorization up to 71.8% due to the insufficient PS dosage, while a decline of OG decolorization was observed as well when PS/Fe(II)/hydroxylamine = 80/10/16 because of the intensive consumption of hydroxylamine and hydroxyl radicals ( OH) by excessive PS. The radicals characterization via electron spin resonance (ESR) technique was also conducted and the results indicated hydroxyl radicals were the predominant oxidative species in studied processes.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）