TALANTA
·
2024
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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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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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
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
·
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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WATER RESEARCH
·
2024
·
IF 11.4
Suhua Gu,Fangshu Qu,Dan Qu,Zhongsen Yan,Yuchuan Meng,Ying Liang,Haiqing Chang,Heng Liang
Membrane distillation (MD) offers promise for recycling shale gas produced water (SGPW), while membrane fouling is still a major obstacle in standalone MD. Herein, sodium percarbonate (SPC) oxidation was proposed as MD pretreatment, and the performance of the single MD, SPC-MD hybrid process and Fe(II)/SPC-MD hybrid process for SGPW treatment were systematically evaluated. Results showed that compared to raw SGPW, the application of SPC and Fe(II)/SPC led to the decrease of the fluorescent organics by 28.54 % and 54.52 %, respectively. The hydrophobic fraction decreased from 52.75 % in raw SGPW to 37.70 % and 27.20 % for SPC and Fe(II)/SPC, respectively, and the MD normalized flux increased from 0.19 in treating raw SGPW to 0.65 and 0.81, respectively. The superiority of SPC oxidation in reducing the deposited membrane foulants and restoring membrane properties was further confirmed through scanning electron microscopy observation, attenuated total reflection fourier transform infrared, water contact angle and surface tension analyses of fouled membranes. Correlation analysis revealed that hydrophobic/hydrophilic matters and fluorescent organics in SGPW took a crucial role in MD fouling. The mechanism of MD fouling mitigation by Fe(II)/SPC oxidation was attributed to the decrease in concentrations and hydrophobicity of organic by synergistic oxidation, coagulation and adsorption.
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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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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Katam Srinivas,Zhuo Chen,Anran Chen,He Huang,Chengtao Yang,Fei Wang,Ming-qiang Zhu,Yuanfu Chen
Replacing platinum-based electrocatalysts with iron single-atom catalysts (Fe–N4–C) for the oxygen reduction reaction (ORR) remains challenging due to the symmetric electronic structure of atomically dispersed Fe–N4 sites and sluggish kinetics. To address this issue, we introduce Cu–Nx sites and graphene-encapsulated core–shell Fe–Cu nanoalloy (FeCu@G) particles into the Fe–Nx site surroundings through the self-assembly and pyrolysis of a metal–organic framework (MOF). This strategy leverages synergistic interactions with the associated species to modify the uniform electronic structure of Fe single-atom sites, thereby enhancing oxygen-adsorption/desorption kinetics. Density functional theory (DFT) calculations reveal that the incorporation of Cu–Nx sites and FeCu@G nanoalloy particles significantly alters the electronic structure of Fe–Nx sites, leading to improved ORR activity. Consequently, the optimized FeCu-DSAs@CNT, comprising dual single-atom sites (DSAs: Fe–Nx and Cu–Nx) and FeCu@G nanoalloy within MOF-derived nitrogen-doped carbon nanotubes (CNTs), exhibits a significantly improved half-wave potential (E1/2 = 0.91 V) and feasible ORR kinetics (Tafel slope = 48.15 mV dec−1), surpassing the Pt/C benchmark (E1/2 = 0.847 V and Tafel slope = 56.76 mV dec−1). Notably, FeCu-DSAs@CNT shows a 58 mV more positive E1/2 compared to monometallic Fe–SAs@CNT, attributed to synergistic interactions with Cu species. Moreover, it demonstrates excellent power density, specific capacity, and cycling stability in a lab-made zinc–air battery, outpacing the Pt/C-battery. This study addresses gaps in understanding Fe–Nx site interactions with associated species, providing valuable insights for the advancement of Fe–Nx–C electrocatalysts.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2024
·
IF 6.9
Pengfei Yang,Jianhong Bi,Hua Zhang,Zhenyu Wu
Herein, we explored the efficacy of ethylenediaminetetraacetic acid (EDTA) intercalation modified layered double hydroxides (LDHs) composites for removing the anionic dye methyl orange (MO) from aqueous solutions. EDTA intercalated layered hydroxides (EDTA-Mg/Fe LDHs) with a 4:1 Mg/Fe molar ratio have been successfully prepared and thoroughly characterized using SEM-EDS, FTIR, XRD, XPS, UV-Vis and Zeta potential analysis. Batch adsorption experiments were conducted to evaluate the adsorption performance of the innovative adsorbent on MO. The results indicated successful EDTA loading into Mg/Fe LDHs, exhibiting excellent adsorption performance for MO. At pH 6.0, with a 0.03 g adsorbent dose, MO removal exceeded 91.10 % within 90 min, following a pseudo second order kinetic model. The maximum adsorption capacity reached 1207.43 mg/g, fitting well with the Redlich Peterson model. Thermodynamic parameters suggested a spontaneous and favorable adsorption process. Furthermore, we assessed the desorption and regeneration effectiveness of EDTA-Mg/Fe LDHs, emphasizing the importance of developing cost-effective and environmentally friendly adsorbents with practical applications and scientific significance.
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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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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Lianzhong Shen,Lin Wang,Yu Ye,Zhouwei Li,Qizhou Dai
The fabrication of various defects on the surface of metal single-atom catalysts can improve their electrochemical CO 2 reduction reaction (CO 2 RR) ability, and the current mainstream research focuses on the defect modification of heteroatom doping, while there are fewer studies on intrinsic defects on carbon substrates. Herein, a series of catalysts with both Fe-N 4 sites and intrinsic defects were synthesized on the ZIF-8 surface by pyrolytic etching at a suitable temperature under ammonia atmosphere. Electrochemical tests in an H-cell showed that the catalyst achieved CO Faradaic efficiency (FE CO ) of 96.9 % and CO partial current density (J CO ) of 9.088 mA cm −2 at −0.6 V. Through further studies, we introduced a “585” ring structure to describe these intrinsic defects and found that these intrinsic defects on the carbon-based surface can act as active sites to promote CO 2 RR along with the Fe-N 4 sites. This work provides a reference for the study of intrinsic defect-modified single atomic materials.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Bo Qin,Bin Wang,Jiang Li,Tao Wang,Xiaoyi Xu,Li'an Hou
Non-radical catalytic oxidation processes can eliminate refractory pollutants from wastewater containing complex substrates such as dissolved organic matter, but the production of selective non-radicals is challenging during the activation of peroxymonosulfate (PMS). Herein, a novel magnetic carbon-based catalyst (Fe 3 O 4 @CD-8, where 8 represents an annealing temperature of 800 ℃) with N and Fe species as catalytic active sites was fabricated to remediate sulfamethoxazole (SMX)-containing water. It showed excellent SMX removal efficiency and facilitated singlet oxygen ( 1 O 2 ) production. The characterization results revealed that Fe 3 O 4 @CD-8 had a microscopically hierarchical pore structure and an overall core–shell-like structure. Due to its large specific surface area, N-containing species, and Fe nanoparticles, 0.1 g/L Fe 3 O 4 @CD-8 removed almost 100% SMX (24 min) and achieved a 44.1% mineralization (40 min) efficiency in the presence of 0.5 mM PMS. This catalytic system also maintained its removal performance in the presence of inorganic anions and humic acids and over a wide pH range of 3–11, showing good tolerance to various environmental factors. 1 O 2 was confirmed to be the predominant active species for SMX degradation using the Fe 3 O 4 @CD-8/PMS system. Density functional theory (DFT) calculations, intermediate monitoring, and toxicity evaluation demonstrated that SMX was transformed into low-toxicity molecules and completely mineralized into CO 2 and H 2 O. The addition of Fe nanoparticles enhanced PMS adsorption and facilitated the Fe(III)/Fe(II) redox cycle to accelerate the activation of PMS. This study provides new insights and strategies for the controlled production of non-radicals for remediating antibiotic-containing wastewater.
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