Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Yibing Feng,Kun Qiao,Xiaohan Jiang,Huiling Ji,Jiang Meng,Jigang Wang
A photocatalysis–self-Fenton system (PSFs) offers a viable solution to the continuous hydrogen peroxide (H 2 O 2 ) dosing and insufficient Fe 2 + regeneration challenges in conventional Fenton chemistry. An oxygen-doped g-C 3 N 4 microrod (OCNT)-based PSFs was synthesized via a facile oxalic acid-mediated supramolecular self-assembly route, enabling efficient pollutant degradation. In situ H 2 O 2 production was achieved through a two-electron oxygen reduction reaction (2e − -ORR), with photogenerated electrons accelerating Fe 2+ /Fe 3+ cycling and enhancing H 2 O 2 utilization. The system exhibited an apparent rate constant of 0.071 min −1 for tetracycline (TC) removal, 12.2- and 4.2-fold higher than pristine g-C 3 N 4 and a photo-Fenton system, respectively. Density functional theory (DFT) calculations and experimental results indicated that oxygen heteroatom doping increased the molecular dipole moment and optimized the band structure, while the one-dimensional microrod morphology exposed abundant active sites. These synergistic effects facilitated charge-carrier separation, improved interfacial mass transfer, and promoted the two-electron oxygen-reduction pathway, thereby accelerating Fe 2+ /Fe 3+ cycling and hole oxidation. The platform demonstrated broad pH adaptability, strong anti-interference capability, and long-term operational stability. This work provides an effective strategy for on-site H 2 O 2 generation and utilization in photocatalytic–Fenton systems for the degradation of organic contaminants.
研究领域:
环境化学
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材料科学
·
催化
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水处理技术
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物理化学
·
纳米技术
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Peng Zhou,Jing Zhang,Zhaokun Xiong,Yang Liu,Xiaowei Huo,Xin Cheng,Wenshu Li,Feng Cheng,Yongli Zhang
Hydroxylated C 60 Fullerene (Fullerol) induced photochemical production of reactive oxygen species (ROS, e.g. singlet oxygen ( 1 O 2 ) and hydroxyl radical ( OH)) is a slow process, and the role of its surface groups other than high water-solubility is still lack of investigation. In this study, we demonstrate Fullerol can promote Fe(III)/Fe(II) cycles to degrade dimethyl phthalate (DMP) in Fe(III)/H 2 O 2 Fenton system as both an electron donor and an electron-transfer mediator. At acidic condition, the formation of carbonyl and carboxyl via pinacol rearrangement and subsequent keto-enol isomerization can produce cage-opened structure of Fullerol, resulting in the pH-dependent formation of Fe(III)-Fullerol complex. Two pathways of Fe(II) recovery via intramolecular electron transfer of Fe(III)-Fullerol complex to enhance Fe(III)/H 2 O 2 Fenton oxidation were proposed: 1) Fullerol direct reduces Fe(III) into Fe(II) as an electron donor in dark, and it was strongly enhanced under visible light irradiation; 2) Fullerol mediates electron transfer from electron donor (e.g. hydrogen peroxide and organics) to Fe(III) in visible light condition. Furthermore, DMP degradation pathway was proposed based on variation of main intermediates.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Feng Cheng,Peng Zhou,Yang Liu,Xiaowei Huo,Jian Zhang,Yue Yuan,Heng Zhang,Bo Lai,Yongli Zhang
Slow reduction of Fe(III) in iron-mediated Fenton-like systems strongly limits the decomposition of H 2 O 2 to produce hydroxyl radicals ( • OH). Here, we report that graphene oxide (GO) possesses excellent reactivity to enhance the Fe(III)/H 2 O 2 Fenton and photo-Fenton oxidation for degrading chloramphenicol (CAP). EPR analysis and quenching tests reveal that • OH is the primary oxidant for CAP degradation. The characterization analysis and iron species transformation experiments demonstrate that Fe(III) can combine with the functional groups on the GO surface to form GO-Fe(III) complexes. The chronopotentiometry and cyclic voltammogram suggest that GO can donate electrons to Fe(III) via intramolecular electron transfer and promote H 2 O 2 induced Fe(III) reduction by increasing the oxidation capability of Fe(III) due to the formation of GO-Fe(III) complexes, resulting in the strong promotion of the Fe(III)/Fe(II) cycle for producing OH. Moreover, the dark- and vis-GO/Fe(III)/H 2 O 2 systems can effectively degrade CAP at initial pH ranging from 2.0 to 4.7. The reusability and stability of GO were evaluated by performing the cyclic degradation experiments of CAP. The OH induced degradation pathway of CAP was proposed involving three stages, based on intermediates analysis of UPLC-QTOF-MS/MS system. Therefore, the GO/Fe(III)/H 2 O 2 system with or without visible light shows high potential for application in environmental remediation.
研究领域:
环境科学
·
化学
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Afang Wang,Yang Shi,Yang Liu,Wei Li,Heng Zhang,Xiaoqiang Dai,Li Luo,Gang Yao,Bo Lai
Traditional Fenton and Fenton-like processes are affected by the sluggish kinetics of Fe(II) regeneration and Fe(III) accumulation. This research revealed that the degradation efficiency of pollutants was significantly increased by adding Fe(III) to the Vis/PS system. A mechanism is proposed in which photosensitivity pollutants can boost Fe(III) to produce Fe(II) under visible light irradiation. Intriguingly, Fe(III) rapidly combines with LVF in aqueous environments to form Fe(III)-LVF complexes. This research confirms that Fe(III)-pollutant complexes are generated. The proportion of complexes are calculated using mathematical models. Furthermore, the production of Fe(IV) is verified in the Vis/PS/Fe(III) system, which also plays a vital role in boosting LVF degradation. Overall, this study provides comprehensive insights into the degradation mechanism of micropollutants, involving hydroxyl radical ( OH ∙ ), Fe(IV), and Fe(III)-LVF complexes, providing an efficient and green strategy for contaminant removal during wastewater treatment .
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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.
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WATER RESEARCH
·
2020
·
IF 9.13
Panpan Wang,Xiaolin Liu,Wei Qiu,Feihong Wang,Haicheng Jiang,Mansheng Chen,Wei Zhang,Jun Ma
Low cost, green, regenerable catalyst for persulfate activation is the popularly concerned topic for the degradation of persistent organic micropollutants in drinking water . In this work, natural montmorillonite (MMT) saturated with Fe(III) ions was used to activate peroxymonosulfate (PMS) for the degradation of atrazine in raw drinking water. Results showed that the adsorption of atrazine was quickly completed within 1 min and the percentage degradation was finally increased up to 94.1% in 60 min. The d 001 -spacing of MMT was enlarged to 2.91 nm at the most by Fe(III) saturation. Atrazine was adsorbed into the nanoscale interlayer of Fe(III)-saturated montmorillonite (Fe-MMT), where the Fe(III)/Fe(II) cycle was sustainably realized through the accelerated transformation of electrons between Fe(III) and PMS. Meanwhile, the in-situ generated Fe(II) accelerated the decomposition of PMS to further proceed the degradation of atrazine through the oxidation of HO• and SO 4 • - radicals. This nanoconfined effect of PMS activation by Fe(III) was further confirmed through the degradation of various micropollutants in the backgrounds of river water. The selective catalytic oxidation of micropollutants through PMS activation was attributed to the 2D mesoporous structure of Fe-MMT, inhibiting the interlayer adsorption of larger molecular backgrounds (humic acids etc. ). Fe(III)-saturated montmorillonite (Fe-MMT) provided a feasible and scalable method of PMS activation by Fe(III) for the degradation of micropollutants in drinking water.
研究领域:
环境科学
·
催化材料
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yunqi Wang,Peng Zhou,Qingguo Wang,Xiaowei Huo,Xue Huang,Qian Ye,Hao Xu,Guanyu Zhou,Yuhang Liu,Jing Zhang
Hydroxylated fullerene, Fullerol, has applied in many areas because of its high electron affinity and antioxidant potential, while it was few used in wastewater treatment. In this study, the mechanism involved that Fullerol accelerated the regeneration of Fe(II) in the Fe(III)/H 2 O 2 system under dark condition, which was investigated with chloramphenicol (CAP) as a model pollutant. In Fullerol/Fe(III)/H 2 O 2 system, CAP removal was completely achieved at 60 min via a non-photochemical pathway. In addition, the quenching experiments and electron spin resonance (ESR) results indicated that hydroxyl radical ( OH) was the main reactive oxygen species (ROSs). The Fullerol/Fe(III)/H 2 O 2 system had a rate constant of CAP degradation about 5.0 × 10 −2 min −1 , which was about 22 times higher than it in Fe(III)/H 2 O 2 Fenton-like system (2.3 × 10 −3 min −1 ). Fe(II) was ascertained the effective component that was responsible for H 2 O 2 activation to produce OH, which derived from 1) the first pathway: Fullerol complexed with Fe(III) and the redox potential of the complex is much lower than Fe(III)/Fe(II); 2) the second pathway: Fullerol acted as an electron donor to reduce Fe(III) into Fe(II). Moreover, CAP degradation intermediates were identified and its degradation pathways were proposed. This study suggested a new approach for improving the Fe(III)/H 2 O 2 system by accelerating Fe(III)/Fe(II) cycles with Fullerol.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 51
·77851-77863
·
IF 5.19
Jiang Changjin,Zhang Ting,Li Shuhui,Yang Zhaoguang
Fe(III)-chitosan and Fe(III)-chitosan-CTAB composites were prepared using an ionotropic gelation method. Various techniques were used to analyze the morphology, structure, and property of the adsorbents, including SEM, EDS, FT-IR, XPS, and zeta potential. Compared with Fe(III)-chitosan, Fe(III)-chitosan-CTAB was more effective for As(V) adsorption at a wide range of pH (3.0–8.0). The adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB could reach equilibrium in 20 min, and their maximum adsorption capacities were 33.85 and 31.69 mg g ‒1 , respectively. The adsorption kinetics was best described by the pseudo-second-order model ( R 2 = 0.998 and 0.992), whereas the adsorption isotherm was fitted well by the Freundlich model ( R 2 = 0.963 and 0.987). The presence of H 2 PO 4 – significantly inhibited the adsorption of As(V) onto Fe(III)-chitosan and Fe(III)-chitosan-CTAB, and humic acid also led to a slight decrease in As(V) adsorption by Fe(III)-chitosan-CTAB. Over 94% of As(V) at the initial concentration of no more than 5 mg L –1 was removed from real water by the two adsorbents. 1% (w/v) NaOH solution was determined to be the most suitable desorption agent. Fe(III)-chitosan and Fe(III)-chitosan-CTAB still maintained their initial adsorption capacities after five adsorption–desorption cycles. Based on different characterization results, both electrostatic attraction and surface complexation mechanisms played important roles in As(V) adsorption on Fe(III)-chitosan and Fe(III)-chitosan-CTAB.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Hao Xu,Qian Ye,Qingguo Wang,Peng Zhou,Xiaowei Huo,Yunqi Wang,Xue Huang,Guanyu Zhou,Jing Zhang
Developing a low-cost and environmental friendly way to promote the Fe(III)/Fe(II) cycling is crucial to enhance the efficiency of Fenton reaction. In this study, g-C 3 N 4 was introduced into the Fe(III)/H 2 O 2 system as electron donor to accelerate Fe(III)/Fe(II) cycling and improve the degradation of organic pollutants under visible light. The g-C 3 N 4 /Fe(III)/H 2 O 2 /light system can achieve excellent degradation of different kinds of organic pollutants under low Fe(III) and H 2 O 2 dosages. The central composite design (CCD) and response surface methodology (RSM) were applied to evaluate the effects of g-C 3 N 4 dosage, Fe(III) dosage, H 2 O 2 dosage and light intensity on the DMP degradation efficiency. The mechanisms were investigated by quenching experiments and electron spin resonance (EPR) analyses that the photo-generated electrons and O 2 – were responsible to the Fe(III) reduction through interfacial and aqueous pathways, respectively. OH was the dominant reactive radical in the DMP degradation. Moreover, DMP degradation routes were proposed including the elimination of specific groups, the hydroxylation process and the ring-opening reactions. This study demonstrates an economical and green approach which provides a promising direction for the practical application of g-C 3 N 4 based photocatalysis by integrating it with the Fe(III)/H 2 O 2 Fenton process.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Feng Cheng,Peng Zhou,Xiaowei Huo,Yang Liu,Yunxin Liu,Yongli Zhang
The photocatalytic behavior of the graphene oxide (GO) modified Fe(III)/peroxymonosulfate (Fe/PMS) system for bisphenol A (BPA) degradation was investigated. With the addition of GO, a dramatic enhancement of BPA degradation was obtained at pH 3.0 under visible light irradiation. According to ESR analysis and quenching tests, both SO 4 - and OH are responsible for BPA degradation. The characterization analysis demonstrates that Fe(III) can chelate with the oxygenic functional groups on the surface of GO forming a stable GO-Fe(III) complex. The detections of different kinds of Fe species reveal that Fe(III) can be reduced to Fe(II) by GO via intramolecular electron transfer in the GO-Fe(III) complex, and visible light could enhance this process. The Fe(III)/Fe(II) cycle not only occurs on the surface of GO, but also in aqueous solution via homogeneous reactions. In addition, the degradation pathway of BPA was proposed based on the identification of the intermediates using GC–MS and LC-MS techniques.
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AQUA-Water Infrastructure Ecosystems and Society
·
2024
·Vol. 73
·期 8
·1671-1682
·
IF 2.1
Li Dajie,Chu Xiao,Chen Chen,Cheng Jun,Huang Weiwei,Yang Fei,Yi Xuesong
To further investigate the synergistic effects of Fe (Ⅲ) and graphene derivatives with varying degrees of oxidation for photocatalysis, commercial titanium dioxide nanoparticles and graphene oxide were employed as precursors to synthesize the catalyst in this study. Graphene oxygenated derivatives and Fe (Ⅲ)-modified titanium dioxide photocatalysts with different oxidation degrees were prepared using a simple one-step solvothermal method. The results demonstrated that the photocatalytic performance in degrading rhodamine B and sulfamethoxazole was enhanced with an increase in the oxidation degrees of graphene materials. Through the combined action of delocalized conjugated π electrons as electron transfer mediators, Fe (Ⅲ) as an electron trap, and photosensitization reactions, titanium dioxide exhibited exceptional photocatalytic properties with the assistance of graphene derivatives and Fe (Ⅲ) co-catalysts in the degradation of organic compounds. We developed a distinctive and straightforward method for fabricating graphene oxide and Fe(III) co-modified titanium dioxide catalysts. The quantity of oxygen-containing functional groups on the surface of graphene oxide precursors was controlled through thermal reduction. The synergistic impact of graphene derivatives and Fe (III) dual co-catalysts was further enhanced.
研究领域:
材料科学
·
环境科学
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高影响因子
INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Zhi-Kun Liu,Zi-Shuo Yao,Jun Tao
Halogen-substituted Fe(III) compounds, [Fe(HphsalpmX)2]PTFB (HphsalpmX = 5-X-(R,S)-((phenyl(2-pyridyl)methylimino)methyl)phenol, PTFB = phenyltrifluoroborate; X = F for 1, Cl for 2, Br for 3) and [Fe(HphsalpmX)2]PTFB·MeOH (X = I for 4·MeOH), were synthesized. Compounds 1, 4·MeOH, and its desolvated form 4 exhibited an invariant high-spin state in the whole temperature range, while 2 and 3 underwent gradual, nonhysteretic, and incomplete spin crossover (SCO) with transition temperatures (TC) of 153 and 220 K, respectively. Interestingly, the SCO-active compounds 2 and 3 showed light-induced excited spin-state trapping (LIESST) effects at 10 K, and light-induced reversible ON/OFF switching behaviors were realized by alternately using 880 and 1064 nm light, while the thermally inert compound 4·MeOH unexpectedly showed a reverse-LIESST effect. These results may help to design and synthesize new photoresponsive SCO Fe(III) compounds for the development of switchable materials.
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