SENSORS AND ACTUATORS B-CHEMICAL
·
2017
·
IF 5.401
Xiaomin Fu,Yan Yang,Na Wang,Shihong Chen
Here, the cathodic electrochemiluminescence (ECL) behavior of 3,4,9,10-perylenetetracar-boxylic acid (PTCA) coreacted with hydrogen peroxide was firstly reported. The quenching effect of Fe-MIL-88 MOFs (iron based metal-organic framework) on the ECL of PTCA was found, and the ECL quenching mechanism was investigated, which was speculated to be via the resonance energy transfer from PTCA to Fe-MIL-88 MOFs and steric hindrance effect from Fe-MIL-88 MOFs. Combining with dual molecular recognition strategy and the quenching effect of Fe-MIL-88 MOFs on the ECL of PTCA-H 2 O 2 system, an “on-off” ECL sensor was designed to detect dopamine (DA) with a broad linear range (five orders of magnitude). The detection limit was low to 2.9 × 10 −13 M. The PTCA-H 2 O 2 system would provide a new ECL platform, especially for constructing enzyme based ECL sensor with H 2 O 2 as product in enzymatic reaction. Furthermore, the electrochemiluminescence resonance energy transfer between Fe-MIL-88 metal–organic framework and PTCA would expand a new application of Fe-MIL-88 MOFs in ECL field. The dual molecular recognition strategy ensured the selectivity of the sensor for DA detection.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Xin Liang,Laishi Li,Yusheng Wu,Feng Liu,Yuzheng Wang
The efficiency of Fenton-like catalysts was critically affected by the rapid transfer of Fe 2+ /Fe 3+ , a process that was essential for the formation of active free radicals by H 2 O 2 . Herein, we synthesized CuS/Fe 3 O 4 @MIL-100(Fe) (CFM) ternary composites using hydrothermal and in-situ growth methods to enhance the degradation of oxytetracycline hydrochloride (OTC-HCl) in a Fenton-like photocatalytic system. The incorporation of CuS as a co-catalyst into the double iron-based system significantly enhanced photocatalytic activity, achieving a 95.31 % degradation efficiency for OTC-HCl within 50 min under optimized conditions. The catalyst had good reusability, has 86.64 % degradation efficiency after five magnetic recovery cycles, and still showed good catalytic performance in the presence of five different concentrations of common anions. Further analysis using active species quenching and electron paramagnetic resonance (EPR) experiments revealed the role of oxygen-containing radicals in the process. Liquid chromatography-mass spectrometry (LC-MS) and density functional theory (DFT) calculations provided OTC-HCl degradation pathways and intermediates. X-ray Photoelectron Spectroscopy (XPS) analysis indicated that CuS enhanced the performance of the bis-iron-based materials by improving the transfer efficiency of Fe 2+ /Fe 3+ and Cu + /Cu 2+ ions, which in turn accelerated the generation of reactive radicals from H 2 O 2 .
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THERMOCHIMICA ACTA
·
2024
·
IF 3.1
Liang Yu,Lv Shen,Hongzhe Zhong,Ru Zhou,Min Hao,Juncheng Jiang
Polypropylene (PP) flammability poses great fire risks for its application. A metal-organic framework (MOF), NH 2 -MIL-53(Al), was synthesized and subsequently integrated into PP, the flame-retardant efficacy in conjunction with piperazine pyrophosphate (PAPP) and melamine cyanurate (MCA) was additionally examined. When the total mass fraction of the additives was 25 %, the limiting oxygen index (LOI) of PP composite reached 31.1 %, it also passed the UL-94 test with a V-0 rating. The peak heat release rate (pHRR) and the total heat release rate (THR) was reduced by 88.55 % and 79.75 %, respectively, compared with the pure PP. The char residual char percentage increased to 8.02 %. The Tensile Strength reached 30.1 MPa. The results indicate that adding NH 2 -MIL-53(Al) significantly enhanced the flame retardancy and thermal stability of PP composites, without significantly affecting their mechanical properties, which offers a novel potential direction for the advancement of polymer flame retardants (FRs).
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2024
·Vol. 38
·期 9
·e7614
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IF 3.7
Qiuyun Zhang,Feiran Xie,Jialu Wang,Tianqing Wang,Jiao Lei,Weihua Li,Jingsong Cheng,Yutao Zhang
For nearly a century, the excessive discharge of organic contaminants has gradually polluted water and endangered people's health, and photocatalysis has been prominently employed to remove persistent recalcitrant organic. Here, MIL-101(Cr) was firstly employed to introduce thin-layered Bi 2 O 2 CO 3 for the formation of Bi 2 O 2 CO 3 /MIL-101(Cr) nanosheet composite, by a simple and low-temperature in-situ growth approach. The phase, morphology, optical, and surface characteristics of the fabricated composite were characterized through XRD, FTIR, SEM-EDS, N 2 adsorption–desorption, UV–Vis DRS, PL, TG, and XPS techniques, and the ability in the photocatalytic breakdown of rhodamine B (RhB) molecule under visible light was also studied. The results of characterization analysis and optical analysis exhibited that Bi 2 O 2 CO 3 /MIL-101(Cr) has large pore size, good visible light response-ability, and the heterojunction created by intercalating Bi 2 O 2 CO 3 on MIL-101(Cr). Photocatalytic studies revealed that Bi 2 O 2 CO 3 /MIL-101(Cr) had superior RhB degradation activity than pure MIL-101(Cr) and Bi 2 O 2 CO 3 , which achieved 97.1% with visible light irradiation for 20 mg/l RhB. Meanwhile, the Bi 2 O 2 CO 3 /MIL-101(Cr) composite displayed good recyclability after three cycles as revealed by XRD and FTIR analysis proving their excellent stability. This study provides feasible insight into developing novel and efficient MIL-101-based heterojunction catalysts for environmental remediation in the future.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 21
·12712-12720
·
IF 10.7
Tianhao Yu,Peng Gao,Hong Du,Ling Dong
Metal–organic frameworks (MOFs) have recently been reported as promising catalysts for the oxygen evolution reaction (OER). Hence, we chose hydroxyl-rich 2,5-dihydroxyterephthalic acid as the ligand to prepare a novel MIL-100 and wrapped it on the NiCo-ZIF-67 surface to obtain an amorphous hollow material (NiCo-ZIF-67@Fe-MIL-100, denoted as NiCo-ZIF@MIL). The composite material presents a low overpotential (η ≈ 139 mV @ 10 mA cm−2), a small Tafel slope (119 mV dec−1) and great stability for the OER in 1 M KOH solution. Density Functional Theory (DFT) calculations show that the hydroxyl-rich structure, which accelerates OH− transfer and promotes the formation of the Co–O–Fe bridge, effectively reduces the reaction energy barrier (from 2.67 eV for NiCo-ZIF-67 to 2.08 eV for NiCo-ZIF@MIL). This work provides an important reference for the development of double-MOF materials.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2025
·Vol. 39
·期 3
·e70037
·
IF 0
Qiuyun Zhang,Maozhen He,Jialu Wang,Shijian He,Mei Deng,Yanhui Lei,Xiaojuan Zhang,Jingsong Cheng,Zhengjun Liu,Yutao Zhang
The construction and optimization of an effective photocatalyst for photodegradation of persistent recalcitrant organic remains challenging. In this work, MIL-101(Cr)-based nanocomposites (AgI@MCr) are proposed to be fabricated by a simple, green solvent, and room temperature in situ preparation strategy, achieving a highly efficient photocatalytic degradation of organic dye rhodamine B (RhB) molecule under visible light irradiation. Extensive characterization (XRD, FTIR, N 2 adsorption–desorption, SEM and EDS, TG, XPS, UV–vis DRS, PL, transient photocurrent, and EIS) confirmed the composite material's structure, morphology, elemental composition, and optical characteristics. Among all the prepared nanocomposites, AgI@MCr-2 demonstrates outstanding photocatalytic performance for RhB with a removal efficiency of 95.4% within 70 min, and a reaction kinetics of 0.0392 min −1 , superior to pristine AgI or MIL-101(Cr), and also shows excellent durability, retaining over 80% RhB degradation efficiency after four cycles. Remarkably, the significant enhancement is attributed to the built interfacial contact and synergistic effect between substances in the nanocomposite, high specific surface area, strong visible light–harvesting capacity, low bandgaps, and high electron–hole pair separation. In addition, a possible degradation route for the AgI@MCr nanocomposite is further proposed using various analysis techniques. This study provides valuable references for developing effective multicomponent MOF-based photocatalytic composite materials for dyeing wastewater treatment and environmental remediation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yanyu Song,Xianbo Sun,Long D. Nghiem,Jun Duan,Wen Liu,Yongdi Liu,Zhengqing Cai
Building a heterojunction is a fascinating option to guarantee sufficient carrier separation and transfer efficiency, but the mechanism of charge migration at the heterojunction interface has not been thoroughly studied. Herein, MIL-53(Fe)/Bi 4 O 5 I 2 photocatalyst with a Z-scheme heterojunction structure is constructed, which achieves efficient photocatalytic decontamination under solar light. Driven by the newly-built internal electric field (IEF), the formation of Fe-O-Bi electron migration channel allows for rapid separation and transfer of charge carriers at the heterojunction interface, confirmed by the material characterization and density functional theory (DFT) calculation. The narrower band gap and improved visible light response also contribute to the enhanced photocatalytic activity of composite materials. With levofloxacin as the target pollutant, the optimal MIL-53(Fe)/Bi 4 O 5 I 2 achieves complete removal of pollutant within 150 min, the photocatalysis rate of which is ca. 4.4 and 26.0 times that of pure Bi 4 O 5 I 2 and MIL-53(Fe), respectively. Simultaneously, the optimal composite material exhibits satisfactory photodegradation of seven fluoroquinolones, and the photocatalysis rates are as follows: lomefloxacin > ciprofloxacin > enrofloxacin > norfloxacin > pefloxacin > levofloxacin > marbofloxacin. DFT calculations reveal a positive relationship between degradation rate and Fukui index (ƒ 0 ) of main carbon atoms in seven fluoroquinolones. This study sheds light on the existence of electron migration channels at Z-scheme heterojunction interface to ensure sufficient photoinduced carrier transfer, and reveals the influence of pollutant structure on photolysis rate.
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PubMed
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Liyun Zhang,Xin Wen,Qingxia Ming,Xue luo,Tianfeng He,Tian Chen,Minghang Jiang,Mengjun Wang,Lan Ma
With environmental pollution becoming more serious, developing efficient treatment technologies for all kinds of organic wastewater has become the focus of current research. In this work, the coaxial electrospinning technology was used to one-step fabricate a porous and underwater superoleophobic polyacrylonitrile nanofibrous membrane with an Fe-based metal–organic framework (MIL-100(Fe)). Benefiting from the synergistic effect of two jets, the nanofibers are smaller and denser, which prompt the exposure of more nanomaterial additives (MIL-100(Fe)). The BET surface area increased to 202.888 m2/g, and the membranes demonstrated outstanding underwater superoleophobicity. Moreover, compared with traditional blended matrix membranes by the single-axis method, separation of the modifier and membrane matrix material by coaxial methods also maintained excellent mechanical properties, which enhanced Young’s modulus 3.4 times (∼1.34 MPa). As a result, facing soluble dyes, the porous C-PAN/MIL-100(Fe) membrane can demonstrate outstanding and fast adsorptive property (the Qm of MB and CR reached 44.71 and 88.74 mg g–1, respectively). For oily emulsion, the hydrophilic and oleophobic nanofibrous reticular surface provided excellent separation performance (flux: 1124.0–1549.3 L m–2 h–1, R > 98%). Moreover, the porous and underwater superoleophobic C-PAN/MIL-100(Fe)-0.5 membrane can synchronously purify the dye/oil mixture emulsions by one-step filtration. Based on the above performance, we believe that the modified nanofibrous membrane prepared by one-step coaxial electrospinning technology can promote more studies of the development of membrane preparation technology in the field of oily wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Ruina Xuan,Jiwen Chen,Yixin Dou,Zhuo Jiang,Xiaofang Li,Deng Ding,Chunlei Wang,Juntao Yan,Linbing Sun
Dual-co-catalyst-modified photocatalysts enhance charge separation efficiency, but the traditional dual co-catalyst is still difficult to get a high separation efficiency due to size and aggregation. Herein, we report bimetallic MIL-53(Fe/Mn) as dual co-catalysts with separate electron and hole mediators. CdS NPs were in-situ grown into MIL-53(Fe/Mn) at varying ratios. 20 %CdS/MIL-53(Fe/Mn) composites shown optimum photocatalytic CO 2 reduction activity. The XPS results shown the strong interaction between CdS and MIL-53(Fe/Mn). The EPR measure proved the carriers of CdS can be transferred to MIL-53(Fe/Mn) oxidation cluster by the oxo-Fe(III)/Fe(II) and oxo-Mn(II)/Mn(III) redox cycling, and the results also suggest the oxo-Fe(III) and oxo-Mn(II) were redox active sites. We believe the approach that bimetallic MOFs act as dual cocatalyst to improve the photocatalytic activity would open a new avenue for the separation efficiency of photo-generated charge carriers.
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DALTON TRANSACTIONS
·
2025
·
IF 3.3
Yuhang Wang,Guixin Yang,Chao Wang,Hongtao Liu,Xinming Wang,Haijun Pang
Central to the development of electrocatalysts that are cost-effective and highly functional are the synthesis of materials and the meticulous delineation of their morphology. This article introduces a solvent-thermal method for constructing ruthenium-based electrocatalysts (Ru/MIL-53@NF), distinguished by the in situ generation of ruthenium nanoparticles (NPs) on MIL-53 with notable dispersion. The procedure requires precise control over ruthenium integration and results in electrocatalysts with exceptional dispersion properties. Furthermore, the optimally engineered Ru/MIL-53@NF exhibited outstanding electrocatalytic hydrogen evolution performance, registering an overpotential of merely 17 mV at 10 mA cm−2 and a Tafel slope of 53.7 mV dec−1, thus outstripping the standard 20 wt% Pt/C benchmark. This research highlights the careful calibration of synthetic parameters to forge ruthenium-based electrocatalysts with both high efficacy and stability.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Si Duan,Yuan Gao,Guihong Lan,Haiyan Qiu,Bo Xu,Xiangming Liu,Ming Zhang,Yusong Chen
Functionalization of ligands is an effective strategy to enhance the adsorption performance of adsorbents. In this study, MIL-101(Fe)-R (R = -H, –OH, –NH 2 , and –NO 2 ) was selected as a platform for systematically studying the impact of functionalization on the adsorption behavior of chlortetracycline (CTC). A series of characterizations were conducted on the prepared MIL-101(Fe)-R to clarify the influence of organic linkers on the microscopic morphology, pore structure, and surface functionality of the adsorbents. Additionally, the effects of different functional groups on the adsorption behavior of MIL-101(Fe)-R were compared to screen for MOFs with high efficiency in removing CTC. Experimental results showed that the maximum adsorption capacities (q m ) of MIL-101(Fe), MIL-101(Fe)–NH 2 , MIL-101(Fe)–OH, and MIL-101(Fe)–NO 2 were 418.980 mg/g, 559.854 mg/g, 187.387 mg/g, and 154.131 mg/g, respectively. Among them, MIL-101(Fe)–NH 2 exhibited a higher mass transfer rate (reaching equilibrium in 15 min). Based on apparent adsorption behavior, adsorption kinetics, isotherm and thermodynamic studies, as well as FTIR and XPS characterizations before and after adsorption, the performance modulation mechanism of MIL-101(Fe)-R in CTC adsorption was discussed in detail. Combined with density functional theory (DFT) calculations, the host–guest interaction controlling the adsorption behavior was understood at the molecular level, demonstrating the optimal binding sites of the adsorbents. This study provides guidance for the design of efficient MOF adsorbents for antibiotic wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Wei Dong,Chunyan Du,Yin Zhang,Jiao Cao,Jingyi Jiang,Lu Zhou,Guanlong Yu,Yulv Zou,Huaiyuan Peng,Rong Yan,Yu Yang
Visible light-driven photocatalysis often struggles with fast recombination of photogenerated electron-hole pair and unsatisfactory degradation efficiency of hazardous micropollutants, such as antibiotics. Constructing an effective heterojunction can address these challenges. In this study, a novel S-scheme MIL-53(Fe)/FeOCl heterojunction composite was synthesized using a hydrothermal method. Factors influencing oxytetracycline (OTC) removal and the underlying reaction mechanism were investigated. The MF-10 composite demonstrated a remarkable removal efficiency of 90 %, significantly higher than that of MIL-53(Fe), which was 54 %. Even after six cycles, the degradation efficiency only decreased by 8 %, and the composition of MF-10 remained unchanged, indicating excellent durability. The photocatalytic process involves crucial reactive species such as · OH, SO 4 • – , O 2 • – , and h + . The heterojunction construction extends the absorption range of visible light, and the internal electric field enhances the separation of photogenerated electron-hole pairs while maintaining robust electron and hole activity. Additionally, photogenerated electrons facilitate the Fe(II)/Fe(III) cycling, resulting in the production of more reactive species for OTC degradation. This work introduces a novel approach to enhance the activity of photocatalysts and provides valuable insights into the design of peroxydisulfate activators.
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