CHEMOSPHERE
·
2021
·
IF 7.086
Hang Liu,Hua Yin,Minghan Zhu,Zhi Dang
Organophosphorus flame retardants (OPFRs) have been regarded as one of the most rebarbative classes of emerging contaminants due to their persistence and toxicity. In the current study, Fe-based metal organic framework (MIL-88A) was synthesized and employed as photo-Fenton catalyst for the degradation of tris-(2-chloroisopropyl) phosphate (TCPP), a typical representative of OPFRs. The observations indicated that visible light could boost the reduction of ≡Fe III to ≡Fe II in Fe–O clusters of MIL-88A during the photo-Fenton system and consequently induce the transformation of H 2 O 2 to OH, which realized efficient degradation of TCPP. Due to the excellent function of MIL-88A, the effective pH application range of photo-Fenton system was extended in comparison with traditional Fenton system. The degradation efficiency of TCPP was visibly influenced in presence of humic acid (HA). MIL-88A exhibited a commendable reusability and stability after 3 times cycle. As the photo-Fenton reaction proceeded, TCPP was disintegrated to several kinds of carboxylated, dechlorinated and hydroxylated products. The observations of metabolomics endorsed that the interference of intermediate products mixture on E. coli weakened to a certain extent. In conclusion, carboxylation , dechlorination , hydroxylation and oxidation of TCPP were likewise effective for its detoxification, revealing that heterogeneous photo-Fenton system driven by Fe-based metal organic framework will be an attractive and safe treatment technique for OPFRs control.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2024
·
IF 7.7
Bin Nie,Haojun Dong,Jincan Yan,Shengyu Zhang,Shuang Zhong
The activation of peroxymonosulfate (PMS) by heterogeneous catalysts presents an exciting but challenging strategy for degrading persistent organic pollutants in water. Iron oxychloride (FeOCl) is considered a promising heterogeneous catalyst due to its unique oxygen bridge structure, which could render it more active by facilitating the iron valence transitions between Fe(II) and Fe(III). However, the limited Fe(II)/Fe(III) conversion cycle rate hinders its catalytic activity, leading to unsatisfactory PMS activations in practical applications. Herein, we demonstrated the performance and the mechanistic pathway of enhanced FeOCl (CNFeOCl) catalytic activation using a graphitic carbon nitride (g-C 3 N 4 ) with a unique electronic structure as a carrier employing 2,4-dichlorophenol (2,4-DCP) as a representative pollutant. The CNFeOCl/PMS system achieved complete degradation of 2,4-DCP (30 mg/L) in a short time (<5 min), whereas the FeOCl/PMS system degraded only 35.98% under the same conditions. The high 2,4-DCP degradation rate of CNFeOCl was due to its improved Fe(II)/Fe(III) ratio (34.34%/40.03%), increased specific surface area (30.32 m 2 /g), and reduced charge-transfer resistance. Combining a series of characterizations, electron spin resonance (ESR) detection, and quenching experiments, the investigations elucidated the enhanced catalytic activation mechanism of CNFeOCl which includes dominant reactive oxygen species (ROS) generation and some key factors that generally affected the efficiency of oxidative degradation. We believe this study offers new insights into the intrinsic role of g-C 3 N 4 supported FeOCl for PMS activation and provides theoretical support to guide the rational design for developing efficient iron-based catalysts toward heterogeneous catalysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Xuecong Qian,Shilong Wang,Haijun Cheng,Luwei Li,Yun Liu,Jinhao Duan,Da Wang,Jun Ma
Fe(II) and Mn(II) are abundant in groundwater and require operationally simple and efficient method to remove in drinking water treatment. The rapid oxidation of Mn(II) is essential in water treatment. This study investigates the efficiency of Mn(II) oxidation by free chlorine in the presence of Fe(II). The results demonstrate that the presence of Fe(II) significantly accelerates the oxidation rate of Mn(II) by free chlorine under neutral and alkaline conditions. The rapid oxidation of Fe(II) by free chlorine and the presence of Mn(II) promote the formation of in situ Mn(II)-doped ferrihydrite. Kinetic modeling and characterization of Fe(III) oxides confirm that the heterogeneous catalytic effect of the Mn(II)-doped ferrihydrite, rather than manganese oxides or their coupled catalytic effect, is responsible for the enhanced oxidation rates. The doped Mn(II) substitutes the tetrahedral Fe(III) ions in the ferrihydrite, introducing additional negative charges at the doped sites. The increased charge enhances Mn(II) adsorption and lowers its redox potential, thereby accelerating Mn(II) oxidation rate through direct electron transfer with adjacent free chlorine. Additionally, the lepidocrocite formed by the reaction between Fe(II) and dissolved oxygen significantly impedes the catalytic performance. These findings provide new insights into the catalytic co-oxidation mechanism of Fe(II) and Mn(II), and help the optimization of water treatment engineering practices.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
✓ 已验证
产品关联
DOI
高影响因子
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Huijuan Cai,Yalin Zhu,Huilin Xu,Hetao Chu,Dongyue Zhang,Jianshu Li
Considering that detection on cations or ions still meets some challenges in achieving the effectivity and selectivity just by employing one platform, the ingenious fabrication of nanomaterials exhibits an increasing research interests for the preponderance in improving or integrating the performance of single platform. Herein, a fluorescent hybrid nanomaterials based on an organic dye 4-methylumbelliferone (4-MU) as modifier and D -arginine as carbon cores has been developed via a facile one-step hydrothermal synthesis , forming carbon dots (CDs)/4-MU hybrid nanomaterials (CDs-4-MU). This kind of nanomaterials can improve the sensitive and selective detection of single CDs towards Fe 3+ ions in different matrices. The detection mechanism of CDs-4-MU towards Fe 3+ can be attributed to an electron transfer process between CDs-4-MU and Fe 3+ , leading to the fluorescence quenching . The limit of detection (LOD) and corresponding linear range in tris-HCl buffer solution are 0.68 μM and 2.29–200 μM, respectively. Furthermore, this nanomaterial can also achieve a detection of Fe 3+ ions in real samples such as tap water, culture medium and fetal bovine serum. In particular, CDs-4-MU exhibits a good biocompatibility and can be uptaken by MC3T3 cells, thus can be applied for Fe 3+ ions detection in cellular level and cellular imaging. Therefore, this work provides a versatile strategy for the synthesis of CDs-based hybrid nanomaterials and opens a new pathway for improving the ion detection in real samples, which is of significance in practical applications.
✓ 已验证
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiamin Wei,Qing Wang,Mian He,Shuai Li,Yunan Zhang,Yang Yang,Shipeng Luo,Lianshe Fu,Xin Wang,Tinghai Yang
The development of highly efficient strategy to facilitate comprehensive charge transmission and effective spatial charge separation is expected as a promising approach to improve photocatalytic performance. Herein, the Fe(III) doping modified AgI/NH 2 -MIL-68(In/Fe) Z-scheme heterojunction (ANM-x composite) with unique internal and interfacial charge transmission performance was fabricated by a facile ion exchange precipitation method. The optimized ANM-50 composite exhibits the maximum photocatalytic activity for the degradation of tetracycline, which is about 9.54, 2.61 and 1.86 times higher than that of pure NH 2 -MIL-68In, NH 2 -MIL-68(In/Fe) and AgI, respectively. The characterization results displayed that Ag nanoparticles (NPs) were generated during the photocatalytic procedure, which not only served as a charge transfer-highway, but also reduced the charge flow energy barrier, thereby accelerating charge transfer efficiency and consolidating the stability of the Z-scheme heterojunction. Mechanism exploration reflected that the superior photocatalytic performance was associated with synergetic effect among the introduced Fe(III), constructed ANM Z-scheme heterojunction and the generated Ag NPs, which significantly expands visible light response range and promotes more effective internal and interfacial charge separation. This research not only designs an efficient photocatalyst for decomposing tetracycline, but also opens a new perspective for rational developing Z-scheme heterojunction with unique internal and interfacial charge flow steering.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Hugang Li,Yongfei Gao,Hongxu Chen,Hui Zhou,Yuhong Qin,Shuai Niu
Addressing the challenges associated with phosphorus and arsenic coexistence is not only a scientific necessity but also a practical imperative for the growing importance of sustainable sewage sludge management. This study investigates the speciation and crystallization transformations of phosphorus and arsenic in sewage sludge under Fe(III)-catalyzed hydrothermal treatments with pH ranging from 2.5 to 8.5. Arsenic and phosphorus, both belonging to the same group of the periodic table, exhibit dynamic interactions during Fe(III)-catalyzed hydrothermal treatments. Results reveal that hydrochar yield decreases with lower pH, while the proportion of arsenic(V) in hydrochar decreases with increasing calcium ion concentration. Scanning electron microscopy shows that fibrous and needle-like structures on hydrochar surfaces enhance the adsorption and enrichment of dissolved phosphorus and arsenate, forming vivianite-P and vivianite-like mineral phases. Notably, the crystallization of scorodite (FeAsO 4 ·2H 2 O) facilitates the immobilization of As(III) in near-neutral environments. These findings deepen our understanding of the synergistic morphological processes and crystallization transformations of arsenic and phosphorus during Fe(III)-catalyzed hydrothermal treatments, offering significant implications for P-rich biochar fertilization and application.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Chenrui Liu,Yun Liu,Zhi Dang,Shuai Zeng,Chengcheng Li
In this paper, a kind of novel core-shell structured heterogeneous photo-Fenton catalyst, boron-doped reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @B-rGO) composite, was successfully synthesized by heating the mixture of Borane-Tetrahydrofuran adduct and graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @GO) under reflux conditions. The core-shell structure of the catalyst had been confirmed by X-ray diffraction (XRD), Raman spectroscopy, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photo electron spectra (XPS), and electron energy loss spectrum (EELS). The experimental results for Bisphenol A (BPA) degradation demonstrated that the as-prepared catalyst exhibited much higher photo-Fenton catalytic activity than Fe 3 O 4 and reduced graphene oxide wrapped Fe 3 O 4 (Fe 3 O 4 @rGO). Additionally, Fe 3 O 4 @B-rGO with mass concentration of doped boron at 9.3% exhibited the optimum catalytic property, in which system the BPA degradation kinetic rate constant was almost 1.96 times and 1.82 times of that in the systems with Fe 3 O 4 and Fe 3 O 4 @rGO, respectively. Finally, the mechanism analyses verified that OH, O 2 − and h + were the main reaction species in this system, and photo-electron generated by boron doped reduce graphene oxide (B-rGO) can accelerate the redox between Fe(II) and Fe(III). The excellent photo-Fenton performance, stability and magnetic separation properties make it promising for the degradation of organic compounds in waste water under visible light.
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 4.3
Ruxin Liu,Tao Yu,Xingwang Niu,Jinsheng Li,Xuefei Lei,Zhaobo Wang,Rui Guo
Antibiotic pollution from compounds such as tetracycline hydrochloride (TC-HCl) is a growing concern due to its persistence in the environment and potential to promote antimicrobial resistance. Conventional treatment methods for such wastewater often suffer from low efficiency and high operational costs. In this study, a bimetallic FeMn-BTC material with a two-dimensional sheet-like morphology was synthesized via a facile one-pot ultrasonic method for the efficient degradation of TC-HCl. By precisely selecting the Fe/Mn molar ratio to 7:3, a high density of accessible Fe(II) active sites was achieved. Under visible-light irradiation, FeMn-BTC degraded 92% of high-concentration TC-HCl (100 mg/L) with a reaction rate constant of 0.06703 min −1 , which is 10.5 times higher than that of the monometallic Fe-BTC. This remarkable enhancement is attributed to the incorporation of manganese, which facilitates the Fe(III)/Fe(II) redox cycle and extends the visible-light absorption range. Density functional theory (DFT) calculations further verify that manganese doping lowers both the adsorption and O-O bond cleavage energy barriers of H 2 O 2 . Mechanistic studies identify hydroxyl radicals (·OH) as the primary reactive species, with the synergistic interaction between iron and manganese promoting H 2 O 2 activation and charge-carrier separation. The catalyst also exhibits excellent stability over a wide pH range (3–9) and shows universal degradation activity toward various pollutants (methylene blue, rhodamine B, and malachite green) as well as in real water matrices containing common anions such as Cl − and SO 4 2− . After four consecutive recycling runs, the material retains over 75% of its initial degradation efficiency, outperforming most reported metal–organic framework-based catalysts. This work offers theoretical insights and a practical strategy for designing highly efficient photocatalysts for Fenton-like reactions.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu
Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 18
·7055-7074
·
IF 8.307
Rutong Song,Jun Yao,Mei Yang,Zhongbin Ye,Zhuang Xie,Xiang Zeng
Water pollution control is one of the major challenges currently faced. With the development of photocatalytic technology, an increasing number of new and efficient catalysts have been developed, but most of the catalysts have limited light capture ability and catalytic degradation efficiency. Therefore, in this work, hydrogen peroxide was further introduced to establish a photo-Fenton system to improve the photocatalytic effect by constructing a Z-scheme, and the degradation ability of the catalyst was maximized. Moreover, we successfully adhered bismuth tungstate nanosheets onto the surface of a MIL-101(Fe) framework and changed the number of active sites with iron ions of different doping amounts. We found that the number of active sites in the photo-Fenton system does not increase linearly, but increases and decreases regularly, which is similar to the change in band structure after doping. In addition, the results of the radical scavenger experiment and electron paramagnetic resonance (EPR) revealed that both hydroxide radical (˙OH) and superoxide radical (˙O2−) participated in methylene blue (MB) degradation, of which ˙OH was the main active species for pollutant degradation. Based on high-performance liquid chromatography-mass spectrometry (HPLC-MS) analysis, the possible degradation pathways were proposed. We believed that this work will provide insights into the heterojunction photo-Fenton system.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）