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
·
2022
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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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Jiandong Guo,Husheng Jia,Aiqin Zhang,Zhen Pei,Man Luo,Jinbo Xue,Qianqian Shen,Xuguang Liu,Bingshe Xu
Iron-based MOFs have been considered as the candidate for Fenton-like reagents owing to their open pore size and uniformly dispersed Fe active centers. However, the strong coordination of metal ions with organic ligands greatly reduces the exposed active sites of most iron-based MOFs, thus reducing Lewis acid sites and limiting the activation efficiency of H 2 O 2 . At the same time, low Fe 3+ /Fe 2+ cycle efficiency also restricts H 2 O 2 activation efficiency. Hence, in this work, a series of MIL-100 (Fe) containing mixed valence coordinatively unsaturated metal site (CUS) with different Fe 2+ /Fe 3+ ratios was synthesized by heat treatment and used for tetracycline hydrochloride (TC-HCL) degradation with the assistance of visible light. Interestingly, accelerated Fe 3+ /Fe 2+ cycle was observed with the aid of visible light. Among the prepared samples, CUS-MIL-250 prepared under vacuum at 250℃ has superior degradation performance, primarily owing to its large specific surface area and pore volume, improved visible light absorption, and the introduction of more Fe 2+ CUS. Meanwhile, compared with Fenton-like system and photocatalytic system, the CUS-MIL-250/H 2 O 2 /Vis system, with effective separation of photogenerated electrons and holes, demonstrates a synergistic effect to generate more reactive oxidation species, thereby improving the degradation efficiency. In addition, the catalyst shows good stability and recyclability.
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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
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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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CHEMOSPHERE
·
2024
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IF 8.1
Jie Zhang,Xufei Wang,Yiwei Liu,Tao Jin,Liang Liu,Xiaodong Ma,Gengbo Ren
The efficiency and stability of the electrical activation of persulfate (PS) by transition metal-based cathode are controlled by the cycling of Fe(III)/Fe(II) and the mass transfer of PS. In this study, the mixed-valence MOFs catalyst (Fe II -MIL-53(Fe)) modified flow-through cathode was prepared for the first time. Fe II -MIL-53(Fe) was prepared by replacing part of the iron-oxygen network structure in MIL-53(Fe) with Fe(II), resulting in the formation of coordinated unsaturated iron centers (CUICs). The increase of the Fe(III) CUICs facilitated the conversion of Fe(III) to Fe(II). Furthermore, the cycling of Fe(III)/Fe(II) was further promoted by the electric field. Meanwhile, the hydrodynamic behavior of flow-through cathode was indicated by the computational fluid dynamics (CFD) simulation. The quenching experiments and electron paramagnetic resonance (EPR) results showed that several reactive specie (SO 4 ·- , ·OH, O 2 ·- and 1 O 2 ) were produce. In summary, this work provided an effective strategy for the efficient and stable electrical activation of PDS.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xiaohui Lu,Yuantai Li,Shihuai Deng,Yanjun Li,Chenye Fu,Guochun Lv,Da Wang,Junxi Song,Hong Xiao,Jiali Peng,Bo Lai
Iron-activated periodate (PI)-based advanced oxidation technologies remain constrained by critical challenges including the facile oxidative deactivation of Fe(II) and the weak reactivity between Fe(III) and PI. This study developed an oxidation system based on readily biodegradable nitrilotriacetic acid (NTA)-chelated Fe(III) complexes for efficient PI activation. The Fe(III)-NTA complex significantly enhanced the reactivity of Fe(III) toward PI, enabling complete degradation of carbamazepine (CBZ, 20 μM) within 60 min. Mass spectrometry identified hydroxylation, ring cleavage, and decarboxylation as primary degradation pathways for CBZ. Results from quenching experiments, chemical probe tests, electron paramagnetic resonance (EPR), 18 O isotopic labeling, and mass spectrometry collectively demonstrated that high-valent iron-oxo species (Fe(V)-oxo) served as the dominant reactive species, assisted by synergistic hydroxyl radical ( • OH) participation. Experimental and density functional theory (DFT) results indicated that the Fe(III)–NTA complex activates PI via an oxygen atom transfer (OAT) pathway, generating reactive Fe(V)-oxo intermediates. This Fe(V)-oxo species may subsequently undergo single electron transfer (SET) to produce • OH. In the degradation of CBZ, Fe(V)-oxo species and • OH were found to contribute approximately 90.9 % and 9.1 %, respectively. Furthermore, pollutants containing strong coordinating groups or lone pair electron donors exhibited competitive coordination effects with the central Fe atom, hindering Fe(III)-NTA-PI interactions and thereby impeding degradation kinetics. Post-degradation, PI was exclusively converted to non-toxic iodate without reduced iodine species (e.g., hypoiodous acid (HOI), iodine (I 2 ), or triiodide (I 3 − )). Theoretical toxicity simulations indicated significantly reduced ecological risks of transformation products. Acute toxicity assays using luminescent bacteria confirmed moderate alleviation of CBZ product toxicity after Fe(III)-NTA-PI treatment. This work provides novel strategies for optimizing iron-activated PI systems, advancing mechanistic insights into chelation-regulated metal activation, pollutant competitive coordination effects, and structure-activity relationships.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Zhenyu Yan,Wenyu Gao,Chenkai Zhong,Qiangqiang Jiao,Shujie Tian,Jia Liu
Ammonia (NH 3 ) plays an important role in agricultural production and is also an ideal zero-carbon energy source in sustainable hydrogen economy. Electrocatalytic nitrate (NO 3 - ) reduction reaction can simultaneously consume nitrogen pollutants in water during the synthesis of NH 3 , which is the most promising and gentle alternative process to the Haber-Bosch. However, due to the interference of hydrogen evolution reaction and high overpotential, the development of efficient directional ammonia conversion catalysts has become the key. In this study, Mo-Fe 2 O 3 material were fabricated by crystal face engineering and orbital manipulation strategies. The (001) face of α-Fe 2 O 3 with the best electrochemical performance was exposed by thermodynamic control, and the in-situ substitution of Mo single atoms for near-surface Fe atoms was further used to achieve excellent ammonia synthesis activity. NH 3 yield of 493.67 μg/h/mg cat and Faraday efficiency of 95.0% were achieved at -0.5 V vs. RHE (pH=7, 0.1 M PBS+500 ppm NO 3 - ). The mechanistic analysis showed that the highly electronegative Mo atoms induced strong interaction by Fe-O-Mo bond, which prompted Fe(III) to preferentially fill the lower t2g orbital and form a low-spin state. The weaker anti-bonding state enhances the interaction between Fe(III) and the coordinating O atoms in NO 3 - , thereby strengthening electron transfer. In summary, the targeted regulation of the crystal facet and electronic orbitals of catalysts presents a promising strategy for enhancing the conversion of NO 3 - to NH 3 .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Rong Li,Yiziqi Lu,Meiqian Lu,Yue Liu,Guodong Zhang,Qiuling Ma,Jian Zhou,Tiecheng Wang
Iodinated X-ray contrast media, as a frequently used medical diagnosis in the imaging of internal organs, soft tissues, and blood vessels, are widely encountered in water environments because of their non-metabolic ability. Herein, a series of co-precipitates (DBC-FeO x ) of dissolved black carbon (DBC) and FeO x were successfully synthesized. The chelation of Fe species with COO – groups in DBC enhanced the excellent electron transfer capability and persulfate (PS) activation performance of the resulting DBC-FeO x , thus boosting iopamidol (IPM) degradation. The IPM removal rate constant in the DBC-FeO x /PS was 35 times and 4.6 times higher than those observed in the DBC/PS and FeO x /PS systems, respectively. There existed an appropriate C/Fe molar ratio in the DBC-FeO x co-precipitates for PS activation, and the IPM degradation was driven by both radical and non-radical pathways. Fe sites were the primary active sites in DBC-FeO x for PS activation, and C=O groups played an important role in accelerating the Fe(III)/Fe(II) cycle by promoting rapid electron transfer, thereby enhancing radical oxidation pathways. Concurrently, DBC-FeO x acted as an electron shuttle to promote the electron transfer from IPM to PS, creating non-radical pathways for IPM removal. IPM degradation processes involved amide hydrolysis oxidation, hydrogen extraction, and deiodination. The typical iodine species HOI was also converted to non-toxic IO 3 - after IPM decomposition, thus reducing potential risks.
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Nanoscale Advances
·
2020
·Vol. 2
·期 4
·1483-1492
·
IF 0
Honggang Yin,Die Gao,Yan Qiu,Gaoyi Yi,Jun Li,Yingying Dong,Kailian Zhang,Zhining Xia,Qifeng Fu
In recent years, photoluminescent (PL) carbon dots (CDs) have attracted enormous attention because of their many fascinating properties. However, the traditional synthesis routes of PL CDs usually suffer from relatively low quantum yields (QYs) and require complicated operation processes as well as lots of externally supplied energy. Herein, we report a room temperature, green, ultrafast and energy-efficient route for large scale synthesis of highly PL N, S-codoped CDs without any external energy supply. The N, S-codoped CDs are prepared through a novel carbon source self-heating strategy, using the sole precursor tetraethylenepentamine (TEPA) simultaneously as the carbon, nitrogen and heat source, triggered by the heat initiator sodium persulfate (Na2S2O8). The large amount of heat released from Na2S2O8-triggered oxidation of TEPA could effectively promote the spontaneous polymerization and carbonization of TEPA precursors themselves as well as the in situ co-doping of sulfur, which had marked synergistic effects on the fluorescence enhancement of CDs, eventually leading to the high-yield (58.0%) preparation of highly fluorescent N, S-codoped CDs (QY 26.4%) at room temperature within 2 min. Moreover, the fluorescence of N, S-codoped CDs could be selectively quenched by Fe3+ ions in the presence of EDTA, in an ultra-wide range of 0.2–600 μM, with a detection limit of 0.10 μM. Ultimately, the fluorescent nanoprobe was successfully used for the quantitative detection of Fe3+ in human serum samples, indicating its great potential for sensing and biomedical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Haidong Li,Han Song,Yuankun Yang,Haitao Wang,Beibei Fan,Juncheng Zheng,Weiguo Tu,Xuemei Luo,Shu Chen
Efficient and economical reduction and elimination of co-pollution of vanadium (V) and chromium (Cr) from water sources is a major challenge. In this study, sulphate green rust (GR SO4 ) was successfully prepared by co-precipitation method and used for the removal of V(V) and Cr(VI). The findings from batch adsorption experiments indicated that the adsorption capacity of GR SO4 for V(V) and Cr(VI) individually was 30.66 mg⋅g −1 and 39.48 mg⋅g −1 , respectively, with equilibrium reached in 25 min and 10 min. Intriguingly, in a binary system with both V(V) and Cr(VI) present, the time to reach adsorption equilibrium for V(V) removal by GR SO4 was 30 % shorter comparison to the single system under identical conditions. By analyzing the surface characteristics, crystal structure and elemental valence changes of GR SO4 minerals before and after the reaction, it can be obtained that: i) Direct adsorption mainly drives the removal of V(V) by GR SO4 , whereas the removal of Cr(VI) is preceded by reduction and followed by adsorption. ii) In a binary coexistence system, the formation of Fe(III)-Cr(III) oxide (GR-Cr(III)) during the removal of Cr(VI) by GR SO4 formed during the removal of Cr(VI) by GR SO4 creates additional adsorption sites for V(V), which shortens the equilibrium time of the V(V) removal reaction by GR SO4 and reduces the amount of V(V) leached. These findings are of great practical significance for understanding the mechanism and practical application of GR SO4 in the synergistic removal of V(V) and Cr(VI) heavy metals and provide valuable insights into their geophysical-chemical cycling.
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BIORESOURCE TECHNOLOGY
·
2012
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IF 4.98
Xiaoyan Wang,Zuoming Zhou,Guohua Jing
Magnetic poly(styrene–glycidyl methacrylate) porous microspheres (MPPM) with high magnetic contents were prepared by surfactant reverse micelles and emulsion polymerization of monomers, in which the well-dispersed Fe 3 O 4 nanoparticles were modified by polyethylene glycol (PEG) and oleic acid (OA) respectively. The characterizations showed that both of the OA–MPPM and the PEG–MPPM were ferromagnetic, however, the OA–MPPM was used to immobilize the bacteria for more advantages. Therefore, the effects of monomer ratio, surfactant, crosslinker and amount of Fe 3 O 4 on the structure, morphology and magnetic contents of the OA–MPPM were investigated. Then, the OA–MPPM was utilized to immobilize Klebsiella sp. FD-3, an iron-reducing bacterium for Fe(III)EDTA reduction applied in NO x removal. Compared with free bacteria, the immobilized FD-3 showed a better tolerance to the unbeneficial pH and temperature conditions.
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