APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xianhu Long,Zhaokun Xiong,Rongfu Huang,Yahan Yu,Peng Zhou,Heng Zhang,Gang Yao,Bo Lai
Herein, an electrochemical (EC) system was applied as “co-catalyst” to enhance the activation of peroxymonosulfate (EC/Fe(III)/PMS) for efficient Sulfamethoxazole (SMX) degradation. The cathodic reduction reaction can facilitate electron transfer to Fe(III) and trigger the sustainable Fe(III)/Fe(II) redox cycle. Unexpectedly, in addition to hydroxyl radical ( OH) and sulfate radical (SO 4 •− ), non-radicals mechanism including singlet oxygen ( 1 O 2 ) and Fe(IV) were also found involved in EC/Fe(III)/PMS system. The degradation of SMX in EC/Fe(III)/PMS system was accomplished by the collaboration of radicals and non-radicals oxidation . The generation routes and mechanisms of involved reactive oxygen species (ROS) were explored. The relative contributions of OH, SO 4 •− , and nonradical species for the degradation of SMX were calculated to 4.75 %, 25.31 %, and 69.94 %, respectively. Besides, multiple degradation pathways of SMX were proposed by identifying the formed byproducts. The EC/Fe(III)/PMS process could efficiently degrade SMX under the influence of co-existing ions and inactivate pathogens in the wastewater.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2020
·Vol. 21
·期 15
·5347
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IF 4.556
Xiao-Ran Jing,Huan Liu,Yao Nie,Yan Xu
Fe(II)/2-ketoglutarate-dependent dioxygenase (Fe(II)/2-KG DO)-mediated hydroxylation is a critical type of C–H bond functionalization for synthesizing hydroxy amino acids used as pharmaceutical raw materials and precursors. However, DO activity requires 2-ketoglutarate (2-KG), lack of which reduces the efficiency of Fe(II)/2-KG DO-mediated hydroxylation. Here, we conducted multi-enzymatic syntheses of hydroxy amino acids. Using (2s,3r,4s)-4-hydroxyisoleucine (4-HIL) as a model product, we coupled regio- and stereo-selective hydroxylation ofl-Ile by the dioxygenase IDO with 2-KG generation from readily availablel-Glu byl-glutamate oxidase (LGOX) and catalase (CAT). In the one-pot system, H2O2significantly inhibited IDO activity and elevated Fe2+concentrations of severely repressed LGOX. A sequential cascade reaction was preferable to a single-step process as CAT in the former system hydrolyzed H2O2. We obtained 465 mM 4-HIL at 93% yield in the two-step system. Moreover, this process facilitated C–H hydroxylation of several hydrophobic aliphatic amino acids to produce hydroxy amino acids, and C–H sulfoxidation of sulfur-containingl-amino acids to yieldl-amino acid sulfoxides. Thus, we constructed an efficient cascade reaction to produce 4-HIL by providing prerequisite 2-KG from cheap and plentifull-Glu and developed a strategy for creating enzymatic systems catalyzing 2-KG-dependent reactions in sustainable bioprocesses that synthesize other functional compounds.Keywords:Fe(II)/2-ketoglutarate-dependent dioxygenase;2-ketoglutarate generation;regio- and stereo-selective synthesis;hydroxy amino acids;sequential cascade reaction
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CHEMICAL ENGINEERING JOURNAL
·
2018
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IF 6.735
Amina,Xiongyuan Si,Kang Wu,Youbin Si,Balal Yousaf
In this study, a modified Fenton system using calcium peroxide (CaO 2 ) powder, as an effective source of hydrogen peroxide (H 2 O 2 ), for the degradation of sulfamethoxazole (SMX) in aqueous solution was investigated. Our results indicated that degradation of SMX in Fe(II)-EDTA catalyzed CaO 2 system was readily more efficient than in Fe(II) catalyzed CaO 2 system. The SMX degradation efficiency was found maximum at pH 6.0 and SMX degradation was suppressed as the initial solution pH was increased. Nevertheless overall removal efficiency in this system was favorable near to neutral pH. In addition, it was observed that the higher bicarbonates (HCO 3 − ) contents had a considerable scavenging ability to SMX degradation while low concentration exhibited auspicious role. The presence of chlorides (Cl − ), nitrates (NO 3 − ), sulfates (SO 4 2− ), and humic acid (HA) could improve SMX removal in this Fenton-like system. Furthermore, chemical probe and radical scavenging activity confirmed the formation of hydroxyl (HO ) and superoxide (O 2 − ) radicals, and also described that the SMX degradation was predominantly due to the HO -induced oxidative destruction. Electron paramagnetic resonance (EPR) studies for different systems, different pH values and different reaction times were carried out to determine the HO radical intensities. EPR results showed that HO intensities were higher in Fe(II)-EDTA catalyzed CaO 2 system, at pH 6.0 and at 90 s reaction time, respectively. Intermediate products of SMX were identified and possible mechanism of SMX degradation was suggested. In conclusion, this work provided comprehensive knowledge for the use of Fe(II)-EDTA catalyzed CaO 2 system for remediation of SMX contaminated sites.
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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.
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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.
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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.
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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.
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Journal of Environmental Chemical Engineering
·
2020
·
IF 4.3
Meesam Ali,Xiang Zhang,Ayesha Idrees,Muhammad Tariq,Muhammad Danish,Usman Farooq,Ali Shan,Xihao Jiang,Jingyao Huang,Shuguang Lyu
This study demonstrated the prolonged benefits of polyvinyl-coated calcium peroxide (PVA@CP) in Fe(II)/nFeS mediated Fenton-like reaction. PVA@CP was prepared by a coating of PVA on calcium peroxide (CP) and synthesized nano-sized iron sulfide (nFeS) was characterized by scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HR-TEM) with energy dispersive spectroscopy (EDS) elemental mapping, X-ray diffractometry (XRD), X-ray photoelectron spectroscopy (XPS), inductively coupled plasma optical emission spectroscopy (ICP-OES) and Fourier transmission infrared (FTIR) techniques. Trichloroethylene (TCE) degradation in various oxic environments (H 2 O 2 , CP, or PVA@CP) was investigated using Fe(II)/nFeS, and the slowest rate constant of 0.031 M −1 min −1 with 91 % TCE removal highlighted the long-lasting effects of PVA@CP. The effect of initial solution pH revealed that the acidic condition was most favorable. PVA@CP system accumulated the least amount (6.34 mg/L) of Fe(III) than H 2 O 2 and CP systems. Electron paramagnetic resonance (EPR) and scavenging tests highlighted that free hydroxyl radicals (HO free ) contributed dominantly in H 2 O 2 system while both free and surface-bound species participated well in CP and PVA@CP systems. Moreover, the insight mechanism of regenerated Fe(II) on the nFeS surface was explored by XPS. Both oxidation and reduction of sulfur were discussed and declared that S(-II) was responsible for regenerating Fe(II). The recycling sample checked the reusability of nFeS, and 98.8 % TCE removal in actual groundwater emphasized that PVA@CP/Fe(II)/nFeS is a viable technique. In conclusion, the PVA@CP/Fe(II)/nFeS system is highly recommended for long-lasting remediation of TCE contaminated groundwater.
研究领域:
环境科学
·
化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xiaolong Hu,Jingyu Bao,Daiwen Chen,Syed Jalil Shah,Sidra Subhan,Wenxue Gong,Wenyuan Li,Xinqi Luan,Zhongxing Zhao :,Zhenxia Zhao
In the photo-Fenton reactions, fast recombination of photoinduced electrons and holes in Fe-based metal–organic frameworks (Fe-MOFs) slows Fe(III)/Fe(II) cycle, which remains big challenge that significantly retards the overall process. Herein, NH 2 -MIL-88B(Fe) (NM88) was modified with 3,5-diaminobenzoic acid (DB) and TPB-DMTP-COF (COF-OMe) to in situ construct NM88(DB) 0.85 /COF-OMe composite that could strongly harvest the visible light for photo-Fenton degradation of sulfamerazine (SMR). With the addition of DB, electron-donating effect of NM88 was strengthened, which then promoted amino groups to react with aldehyde groups (Schiff-base), and thus highly facilitated the interfacial contact between NM88 and COF-OMe. Such modifications increased the degradation rate constants for NM88(DB) 0.85 /COF-OMe to 15.1 and 17.3 times that of NM88 and COF-OMe respectively with good reusability. Moreover, the catalyst exhibited 32–170 times higher degradation kinetics in comparison to other reported catalysts. Results showed that due to the Schiff-base reaction between NM88(DB) and COF-OMe, electron density on Fe(III) was decreased; and the photogenerated electrons of COF-OMe moved to NM88(DB) to reduce Fe(III), thus resulting in the generation of highly active Fe(II) and ·OH species. Furthermore, the main reactive species were determined to be ·OH and ·O 2 – by trapping experiments, and a possible mechanism of the degradation system followed Z-scheme charge transfer.
研究领域:
环境科学
·
材料科学
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高影响因子
DESALINATION
·
2025
·
IF 9.8
Xinyu Yang,Hao Jiang,Zongsheng Hu,Fanju Meng,Bing Hou,Nan Li,Jingwen Pan,Lei Wang
Excessive fluoride (F − ) in water environment seriously endangers ecological security. This study constructed a series of dual-metal loaded biochar adsorbents (CeFe@BC) by modifying cerium-based materials through Fe doping and coupling with straw-derived biochar substrates. Ce 9 Fe 1 @BC 11 exhibited a remarkable F − adsorption capacity of 110.32 mg/g and had broad operational pH range (q e(pH=2 – 12) ≥ 82.61 mg/g). It showed exceptional selectivity and affinity toward F − even in multicomponent systems. The adsorption process was successfully characterized by pseudo-second-order kinetic (R 2 ≥ 0.999) and Temkin isotherm model (R 2 ≥ 0.952), indicating a chemisorption-dominated mechanism. Mechanistic studies revealed that Fe(II) doping maintained the quantity of Ce(III) active adsorption sites through the Fe(II)/Ce(IV) redox reactions, enabling the inverse transformation from Ce(IV) to Ce(III), rather than participating directly in adsorption. This regeneration mechanism increased the number of adsorption active sites of the material by re-reducing Ce(IV) back to Ce(III) during fluoride adsorption or desorption, thereby significantly enhancing adsorption performance. Unlike other anions that adsorb solely via substitution of terminal hydroxyl groups (T-OH) on metal oxides, fluoride onto CeFe@BC exhibited a dual-site adsorption behavior, involving both T-OH substitution and occupancy of bridging hydroxyl (B-OH) sites. Consequently, the T-OH and B-OH groups coordinated with Ce(III) constitute the primary active adsorption sites. The hierarchical porous structure of the straw biochar exposed abundant adsorption sites and also enhanced electron transfer during redox cycles due to its superior conductivity, enabling regeneration of Ce(III) active sites. This work provided a novel strategy for the synergistic structural-functional modulation of high-performance fluoride adsorbents, advancing the rational design of materials for environmental remediation.
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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.
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JOURNAL OF HAZARDOUS MATERIALS
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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 .
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