WATER RESEARCH
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2024
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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
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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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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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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.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2020
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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.
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CHEMICAL ENGINEERING SCIENCE
·
2026
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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
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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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Nanoscale
·
2022
·Vol. 14
·期 18
·7055-7074
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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.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Runliang Zhu,Yanping Zhu,Haiyang Xian,Lixia Yan,Haoyang Fu,Gangqiang Zhu,Yunfei Xi,Jianxi Zhu,Hongping He
The generation of Fe(II) from Fe(III) is the rate-limiting step in the heterogeneous Fenton reaction, and accelerating this step is critical for enhancing the reaction efficiency and also the subject of extensive studies. In this work, the oxidized multi-walled carbon nanotubes (CNTs) were coupled with ferrihydrite (Fh) to synthesize novel and highly efficient heterogeneous Fenton catalysts (CNTs/Fh). Interestingly, the calculated apparent rate constants by 3%CNTs/Fh could reach ∼7.1 times as high as that by Fh, well in agreement with the accelerated decomposition rate of H 2 O 2 , as well as the enhanced generation rate of Fe(II) and hydroxyl radicals in the CNTs/Fh system. The density functional theory calculations and the cyclic voltammograms curves both well indicated that the Fe(III)/Fe(II) redox cycling on CNTs/Fh could be significantly enhanced during the Fenton reaction, from both dynamic (accelerating the electron transfer from H 2 O 2 to Fh) and thermodynamic (lowering Fe(III)/Fe(II) redox potential) aspects.
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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.
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Gels
·
2022
·Vol. 8
·期 6
·331
·
IF 4.432
Jiayan Shen,Shutong Du,Ziyao Xu,Tiansheng Gan,Stephan Handschuh-Wang,Xueli Zhang
Artificial shape-morphing hydrogels are emerging toward various applications, spanning from electronic skins to healthcare. However, the low freezing and drying tolerance of hydrogels hinder their practical applications in challenging environments, such as subzero temperatures and arid conditions. Herein, we report on a shape-morphing system of tough organohydrogels enabled by the spatially encoded rigid structures and its applications in conformal packaging of “island–bridge” stretchable electronics. To validate this method, programmable shape morphing of Fe (III) ion-stiffened Ca-alginate/polyacrylamide (PAAm) tough organohydrogels down to −50 °C, with long-term preservation of their 3D shapes at arid or even vacuum conditions, was successfully demonstrated, respectively. To further illustrate the potency of this approach, the as-made organohydrogels were employed as a material for the conformal packaging of non-stretchable rigid electronic components and highly stretchable liquid metal (galinstan) conductors, forming a so-called “island–bridge” stretchable circuit. The conformal packaging well addresses the mechanical mismatch between components with different elastic moduli. As such, the as-made stretchable shape-morphing device exhibits a remarkably high mechanical durability that can withstand strains as high as 1000% and possesses long-term stability required for applications under challenging conditions.Keywords:organohydrogels;anti-freezing;shape-morphing;tough hydrogels;flexible electronics
研究领域:
材料科学
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柔性电子
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生物医学工程
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聚合物科学
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Rui Wang,Peng Zhao,Ruiquan Yu,Jing Jiang,Ruifeng Liang,Gongyan Liu
The development of antibacterial and catalytic adsorbents is an ideal strategy to simultaneously remove antibiotics, antibiotic-resistant bacteria, and heavy metal ions from wastewater. Herein, a porous and renewable aerogel was prepared as a lightweight adsorbent by using cost-efficient collagen fibers (CF) from the leather industry. Further, the complexes of Fe 3+ ions with gallic acids modified silver nanoparticles (GA@AgNPs) were selected to sufficiently cross-link the hierarchical CF structure based on coordinated complexation, leading to good mechanical property of the resulted aerogel (AgNPs/Fe@CF). Benefiting from the incorporated AgNPs, AgNPs/Fe@CF aerogel exhibited high antibacterial activity against Tetracycline-resistant E. coli and Methicillin-resistant Staphylococcus aureus. Moreover, the cross-linked AgNPs could accelerate the redox cycle of Fe 3+ /Fe 2+ by facilitating electron transfer and thus enhance the activation of peroxymonosulfate to produce more • OH and SO 4 •− radicals. Therefore, this AgNPs/Fe@CF aerogel demonstrated synergetic Fenton-like catalytic degradation efficiency for 5 different antibiotics (over 90 % within 30 min). In addition, abundant hydroxyl and carboxyl groups on collagen fibers endow desired capacity (greater than70 mg/g) to the porous aerogel, which is able to remove Cr (Ⅵ), Ni (Ⅱ), and Pb (Ⅱ). This study explores a new pathway for the construction of multifunctional aerogel materials for enhancing the purification of wastewater.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2018
·
IF 2.88
Jinxia Xu,Zhangjun Bai,Fanlin Zu,Fanyong Yan,Junfu Wei,Saihui Zhang,Yunmei Luo
A convenient, highly sensitive and reliable assay for 2,4,6‑trinitrophenol (TNP) and Fe (III) ion (Fe 3+ ) in the dual spectroscopic manner is developed based on novel carbon dots (CDs). The CDs with highly blue emitting fluorescent were easily prepared via the one-step potassium hydroxide-assisted reflux method from dextrin . The as-synthesized CDs exhibited the high crystalline quality, the excellent fluorescence characteristics with a high quantum yield of ~13.1%, and the narrow size distribution with an average diameter of 6.3 ± 0.5 nm. Fluorescence and frequency doubling scattering (FDS) spectra of CDs show the unique changes in the presence of TNP/Fe 3+ by different mechanism. The fluorescence of CDs decreased apparently in the presence of TNP via electron-transfer. Thus, after the experimental conditions were optimized, the linear range for detection TNP is 0–50 μM, the detection limit was 19.1 nM. With the addition of Fe 3+ , the FDS of CDs appeared to be highly sensitive with a quick response to Fe 3+ as a result of the change concentration of the scattering particle. The emission peak for FDS at 450 nm was enhanced under the excitation wavelength at 900 nm. The fluorescence response changes linearly with Fe 3+ concentration in the range of 8–40 μM, the detection limits were determined to be 44.1 nM. The applications of CDs were extended for the detection of TNP, Fe 3+ in real water samples with a high recovery. The results reported here may become the potential tools for the fast response of TNP and Fe 3+ in the analysis of environmental pollutants .
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