COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Yuanlu Xu,Xin Dong,Yinan Chen,Na Liu,Xinmin Zhang,Chengwen Song,Xinfei Fan
The application of persulfate-based advanced oxidation processes (AOPs) for the removal of emerging pollutants has garnered increasing interest in the field of water pollution control. However, the synthesis of catalysts that simultaneously exhibit stability and exceptional performance is currently facing enormous challenges. In this study, the in-situ growth of nitrogen-doped carbon nanotubes on stratified Fe@RGO substrate was employed to fabricate a novel three-dimensional (3D) composite material for efficient persulfate activation. The innovative design effectively integrated the superior porosity and high conductivity properties of carbon materials, resulting in a unique synergistic effect that facilitated rapid diffusion of reactants and efficient electron transfer. Meanwhile, the incorporation of nitrogen doping can effectively regulate the binding between metal particles and the substrate, thereby enhancing the stability of active sites. This catalyst not only removed SMX ultra-fast in 10 minutes through PMS activation, but also maintained 93% degradation after 5 cycles. A series of radical testing and trapping experiments revealed that the degradation mechanism is primarily dominated by a non-radical pathway. Additionally, electrochemical experiments confirmed that the Fe@RGO/NCNTs with its 3D interconnected layered structure facilitated direct electron transfer. This work demonstrates the broad application prospects of 3D interconnected iron-nitrogen co-doped carbon materials in organic pollution removal.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Linlin Hao,Jingshuang Yan,Jiaoying Guo,Nannan Wang,Ming Zeng
Swine wastewater is a type of highly turbid wastewater with extremly high concentration of COD, NH 4 + , and total phosphorus. To address the drawbacks of commercial coagulants in the pretreatment of swine wastewater, such as loose flocs, slow settling rates, and the inability to remove NH 4 + , a novel Mg-Fe-Al hybrid magnetic coagulant (Mg/Fe/Al-MC) is prepared by using the high-pressure acid leaching (HPAL) technology based on iron tailings waste. Compared to atmospheric acid leaching (AAL), HPAL significantly increased the iron leaching rate from 22 % to 61 %. The specific surface area was increased from 5.1 to 9.2 m 2 /g. The study revealed the synergistic crystallization-coagulation-adsorption mechanism for the purification of swine wastewater. When the dosage of Mg/Fe/Al-MC was 2.5 g/L and pH was 9.0, the removal efficiency of NH 4 + reached 60 % by forming magnesium ammonium phosphate (MAP). Zeta potential results indicated that the coagulation mechanism of Mg/Fe/Al-MC is primarily based on electrostatic neutralization. After maturing Mg/Fe/Al-MC for 60 h, the content of essential polymeric Fe-Al hydroxide complexes [Fe(III)+Al(III)](b) reached 22.7 %. The insoluble porous particles exhibited a significant adsorption capacity, suggesting its important role in pollutant removal. Under the action of an external magnetic field, the settling velocity of Mg/Fe/Al-MC was significantly faster than that of polyaluminum chloride (PAC), with a much higher clear water yield of 75.5 %. This study provides new pathway for the enhanced pretreatment of swine wastewater.
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TALANTA
·
2017
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IF 4.162
Xue Qian Tang,Yi Dan Zhang,Zhong Wei Jiang,Dong Mei Wang,Cheng Zhi Huang,Yuan Fang Li
In this work, Fe 3 O 4 and metal–organic framework MIL-101(Fe) composites (Fe 3 O 4 /MIL-101(Fe)) was demonstrated to possess excellent catalytic property to directly catalyze luminol chemiluminescence without extra oxidants. We utilized Fe 3 O 4 /MIL-101(Fe) to develop a ultra-sensitive quantitative analytical method for H 2 O 2 and glucose. The possible mechanism of the chemiluminescence reaction had been investigated. Under optimal conditions, the relative chemiluminescence intensity was linearly proportional to the logarithm of H 2 O 2 concentration in the range of 5–150 nM with a limit of detection of 3.7 nM (signal-to-noise ratio = 3), and glucose could be linearly detected in the range from 5 to 100 nM and the detection limit was 4.9 nM (signal-to-noise ratio = 3). Furthermore, the present approach was successfully applied to quantitative determination of H 2 O 2 in medical disinfectant and glucose in human serum samples.
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PubMed
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SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Zekun Dong,Jiao Yang,Jie Yao,Yu Tang,Yan Zhang
Electro-peroxone (EP) is an emerging technology that combines electrochemistry and O 3 to remove contaminants. However, conventional carbon cathodes primarily contribute to the synthesis of H 2 O 2 in the system, which may scavenge HO . Herein, a series of Fe-based layered double hydroxides (LDH) was loaded onto graphite felt cathodes to strengthen the removal of organic contaminants. The EP system with CuFe-LDH/GF cathode (EP-CuFe-LDH/GF) demonstrated the highest removal rate (91.2 % within 20 min) of oxalic acid (OA), a typical ozone-resistance substance, approximately twice that of the EP-GF system. HO was identified the main reactive species. A new pathway for O 2 reduction and the generation of HO was found. The loading of CuFe-LDH altered the reduction pathway of O 2 on the GF cathode from 2e − to 1e − or 4e − process. As a result, HO was produced by the combination of O 3 and O 2 − instead of O 3 and H 2 O 2 , which avoided the quenching of HO by H 2 O 2 and enhanced the removal of OA. Moreover, the breaking complexation by O 3 , cathodic O 3 reduction and metal-OH catalyzed O 3 processes also contributed to the HO formation. Furthermore, the system could efficiently remove OA across a broad pH range of 3.0 to 9.0, addressing the poor performance of conventional EP systems under acidic conditions. Overall, the finding of this significant mechanism advances the understanding of organic pollutants removal and broadens the potential applications of EP system.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
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IF 8.1
Zhenyu Yan,Wenyu Gao,Chenkai Zhong,Qiangqiang Jiao,Xiuyun Zhao,Jia Liu
Fe-Nx sites can activate peroxymonosulfate (PMS) in advanced oxidation processes (AOPs) to produce various reactive oxygen species, and have great potential for removing tetracycline (TC), but their formation and catalytic mechanism are rarely studied. Herein, the Fe/N-C catalyst was prepared by crosslinking chitosan (CS) using a coordination complex of Fe 2+ and phenanthroline as the precursor for FeNx. The results of crystal structure, lattice constant, chemical state of N element and structural analysis have demonstrated the successful construction of FeNx sites. The degradation experiments confirmed that the removal efficiency of tetracycline reached up to 90.7 % within 15 min, with a degradation rate of up to 0.184 min −1 . Moreover, the material has exhibited excellent performance in complex water environments and within a broad pH range (pH = 2.30 ∼ 9.88). Mechanism analysis proves that the active substances in the system are 1 O 2 , •O 2 − , SO 4 •− , •OH and Fe IV = O, of which 1 O 2 played the principal role. The FeNx structure is the primary active site, where the redox cycle between Fe 2+ and Fe 3+ , electron transport between pyridinic N, electron-deficient C and PMS produces active components. In addition, based on the various intermediate products detected, two possible TC degradation pathways are reasonably speculated. In this study, the highly active FeNx sites were successfully constructed, and elucidated their activation mechanism towards PMS, which proved the broad prospect of Fe/N-C materials in pollutant degradation.
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MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Haiyan Zhao,Yi Zhou,Shanshan Li,Kemei Shi,Na Li,Min Cui,Cong Zhang
Hydrogen peroxide (H 2 O 2 ) is an important reactive oxygen species, and its abnormal concentration can cause cell distortion and apoptosis, leading to occurrence of various diseases. Therefore, real-time and sensitive monitoring of H 2 O 2 is essential for early disease diagnosis and pathological research. Herein, a novel nanocomposite of Fe-porphyrin covalent organic frameworks decorated with molybdenum disulfide and multi-walled carbon nanotubes (Fe-pCOFs/MoS 2 -MWCNTs), which had glorious enzyme-like activity, was reported for efficient electrochemical detection of H 2 O 2 . The prepared Fe-pCOFs nanosheets with a large specific surface area and fully dispersed Fe 2+ active sites, could enhance mass transfer and atomic utilization, thereby contributing to excellent catalytic efficiency toward H 2 O 2 . The flower-like MoS 2 nanoflakes not only could catalyze the reduction reaction of H 2 O 2 , but also could serve as co-catalyst and form a catalytic cycle with Fe 2+ of Fe-pCOFs, contributing the continuous emergence of catalytic active sites. The highly conductive MWCNTs was employed to promote electron transfer rate. Ultimately, the obtained Fe-pCOFs/MoS 2 -MWCNTs exhibited excellent electrocatalytic activity and conductivity, significantly amplifying the H 2 O 2 response signal. Under the optimal conditions, the sensor had a wide detection range from 20 to 2650 μΜ for H 2 O 2 with a detection limit as low as 2.2 μΜ. Moreover, the sensor successfully recorded trace amounts of H 2 O 2 released from RAW264.7 cells, showing promising application for real-time and sensitive monitoring of H 2 O 2 in clinic or pathological research.
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Journal of Energy Storage
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2024
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IF 8.9
Yunxiao Jia,Bohao Peng,Xinyi Li,Shifang Huang,Xiaosong Zhang,Yulong Ding,Zhu Jiang
Low thermal conductivity is one of the key defects of pristine phase change materials (PCMs) for solar thermal energy storage. Biomass derived carbonaceous matrix, which could be recycled from wide sources, are favourable to incorporate with PCMs for solar thermal storage applications for their highly porous structure and decent thermal properties. Their unique structures get from the grown plants also endue them with diverse properties and functions, such as anisotropic thermal properties for directional heat transfer. However, direct pyrolysis of biomass generally produces amorphous carbonaceous structure that suffers insufficient thermal conductivity. Therefore, this work proposed a simple, rapid, and effective Fe graphitisation route to derive pine wood as graphitic matrix to synthesize multifunctional shape stabilized composite PCM. The Fe graphitisation process has induced the conversion of amorphous carbon to well-ordered graphitic structure. Further elevating the catalytic temperature contributes to a high graphitisation degree up to 89.53 %. With this Fe graphitisation route, the thermal conductivity of PCM composite at its longitudinal direction has increased from 0.545 W · m −1 K −1 to 1.846 W · m −1 K −1 . The solar absorptivity has reached up to 95.60 %. Besides, a high amount of PCM (∼72.26 wt%) was retained by the matrix, offering a high endothermic enthalpy up to 154.2 J/g. In the meantime, the aligned tubular structure of graphitic matrix leads to an anisotropic heat transfer behaviour, displaying a greater thermal conductivity along the longitudinal direction. Therefore, this study has provided a new approach to fabricate high-performance biomass derived graphitic matrix based PCM composite for solar thermal storage applications.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Zhouyang Ma,Jiawei Wu,Fuling Yang,Shuli Wang,Huan Wen,Ligang Feng
Given its initially low activity and difficulty in active phase formation, Fe site regulation is rarely touched in FeNi-based oxygen evolution reaction (OER) catalysts. Herein, the Fe sites regulation and activity deciphering are demonstrated by selective phase transformation taking nitrogen-doped carbon confined FeNi nanoparticles derived from Fe 2 Ni-MIL-MOF pyrolysis as an example; driven by the reduction atmosphere and Kirkendall effect assisted by melamine pyrolysis, some Fe and Ni sites were separated to form metallic Fe and FeNi alloy and the subsequent fluorination process induced the ionic compound FeF 2 formation rather than NiF 2 , offering a good platform to evaluate the influence of active Fe phase for OER catalysis. Theoretical calculations combined with ex-situ and in-situ spectral characterization techniques proved the complete convention of FeF 2 into a high-valent and reactive intermediate state of FeOOH. Considering the stable metallic state of Ni, the largely improved catalytic performance could be attributed to the Fe site regulation and the subsequent synergistic catalysis effect. Compared to the traditional iron-based catalyst, theoretically, the electronic structure of FeF 2 was more conducive to the active FeOOH phase formation and significantly lowered the reaction energy barrier for OER. By addressing the aforementioned problems, low overpotential and good stability for OER catalysts were realized. The current work showed valid proof of the FeNi-based catalysts regulation via Fe sites for energy-relevant catalysis reactions.
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ChemNanoMat
·
2024
·Vol. 10
·期 8
·e202400240
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IF 2.6
Xuetong Xu,Xu Jia,Cong Liu,Jiaolong Qiao,Fuying Wang,Liuxue Zhang,Dan Yang,Yuan Zhang,Xiulian Wang
The photocatalytic hydroxylation of benzene to phenol is an important reaction for the synthesis of fine chemicals and pharmaceuticals. However, the development of efficient and selective photocatalysts for this reaction remains a challenge. Here, a highly active and selective Fe-MOF/2D-montmorillonite (Fe-MOF/MMT) photocatalyst was prepared via an in-situ method for the hydroxylation of benzene to phenol under the visible light irradiation. The Fe-MOF/MMT composite exhibited excellent photocatalytic performance, with phenol yield of 30.3 % and benzene selectivity of 96.5 % within 4 hours. The high activity and selectivity of the Fe-MOF/MMT photocatalyst were attributed to the synergistic effect between the Fe-MOF and MMT, as well as the unique 2D structure of MMT, which facilitated charge separation and transfer. The Fe-MOF/MMT composite also showed good stability and re-used without significant decrease of activity. This study demonstrated that the potential of Fe-MOF/MMT as a highly efficient and selective photocatalyst for the hydroxylation of benzene to phenol and provided an insight into the design of advanced photocatalysts for sustainable chemical synthesis.
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Materials Today Communications
·
2025
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IF 4.5
Zhilei Zhao,Yu Li,Wenlei Zhai,Liuqing Wang,Qianqian Li,Yudan Wang,Meng Wang
The contamination of highly toxic zearalenone (ZEN) in food and the environment poses a serious threat to human safety. However, it is still challenging to establish an efficient, inexpensive and stable ZEN degradation technology. In this study, a Fe single-atom nitrogen-doped porous carbon (Fe-N-PC) was synthesized by high-temperature pyrolysis and used for efficient adsorption and degradation of ZEN. Fe-N-PC showed a high adsorption capacity (q m = 78.2 mg/g) for ZEN, and the Fe-N-PC/peroxymonosulfate (PMS) system could remove 99.39 % of ZEN, in which 1 O 2 played a major role in ZEN degradation. Furthermore, four degradation products of ZEN were identified and possible degradation pathways were hypothesized. For practical applications, Fe-N-PC was applied to remove ZEN from Coix seed extracts, and the results showed that Fe-N-PC was able to detoxify ZEN from Coix seed (92.32 %). Additionally, Fe-N-PC and ZEN degradation products showed low biological toxicity. In a word, the Fe-N-PC/PMS system was used for efficient adsorption and degradation of ZEN, and has been practically applied in complex food matrices, demonstrating Fe-N-PC may be a promising material for the removal of ZEN in the food field.
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TALANTA
·
2024
·
IF 5.6
Shengyuan Zhang,Haiyan Li,Dezhi Yang,Yaling Yang
In the present research, Fe-based metal-organic frameworks (MIL-101(Fe)–NH 2 ) nanoparticles were synthesized by simple solvothermal methods and used to assay Cr(Ⅵ). The MIL-101(Fe)–NH 2 performs dual functions: the 2-aminoterephthalic acid (NH 2 -BDC) ligand endows a strong fluorescence emission, and the Fe metal nodes are able to facilitate the oxidation of 3,3′,5,5′- tetramethylbenzidine (TMB) directly, resulting in the generation of oxidized-TMB (ox-TMB). Our research results showed that reducing agents such as ascorbic acid (AA) can collapse the structures of MIL-101(Fe)–NH 2 because of the reduction of Fe 3+ by AA, resulting in release of NH 2 -BDC. In the presence of Cr(Ⅵ), the fluorescence intensity of the MIL-101(Fe)–NH 2 + AA system will be decreased due to the competitive reduction of Fe 3+ and Cr(Ⅵ). Nevertheless, Cr(Ⅵ) can significantly accelerate the oxidation of TMB by MIL-101(Fe)–NH 2 as it boosts the electron transfer rate between Fe 3+ and Fe 2+ . Therefore, a fluorescent/colorimetric dual-mode platform was developed for the detection of Cr(Ⅵ) with an extensive linear range (7.5–750 μg/L and 13.3–1000 μg/L) as well as a remarkably low detection limit (0.99 μg/L and 1.98 μg/L). This MOF with the ability to release ligands not only provides inspiration for the design of new luminescent materials, but also offers a novel and reliable solution for the detection of Cr(Ⅵ).
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BIORESOURCE TECHNOLOGY
·
2024
·
IF 9.7
Qiushi Jiang,Yanjing Li,Minmin Wang,Wen Cao,Xueying Yang,Sihu Zhang,Liejin Guo
This study investigated the mediating effect of Triethanolamine on Fe@C- Rhodobacter sphaeroides hybrid photosynthetic system to achieve efficient biohydrogen production. The biocompatible Fe@C generates excited electrons upon exposure to light, releasing ferrum for nitrogenase synthesis, and regulating the pH of the fermentation environment. Triethanolamine was introduced to optimize the electron transfer chain, thereby improving system stability, prolonging electron lifespan, and facilitating ferrum corrosion. This, in turn, stimulated the lactic acid synthetic metabolic pathway of Rhodobacter sphaeroides , resulting in increased reducing power in the biohybrid system. The ternary coupling system was analyzed through the regulation of concentration, initial pH, and light intensity. The system achieved the highest total H 2 production of 5410.9 mL/L, 1.29 times higher than the control (2360.5 mL/L). This research provides a valuable strategy for constructing ferrum-carbon-based composite-cellular biohybrid systems for photo-fermentation H 2 production.
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