RSC Advances
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2021
·Vol. 11
·期 18
·10540-10547
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IF 3.361
Anxia Li,Xiaoxin Yang,Juan Chen
Metal–organic frameworks (MOFs), such as MIL-53(Fe), have considerable potential as drug carriers in cancer treatment due to their notable characteristics, including controllable particle sizes, high catalytic activity, biocompatibility and large porosity, and are widely used in a broad range of drugs. In this study, a new approach for the synthesis of MIL-53(Fe) nanocrystals with controlled sizes has been developed using a non-ionic surfactant PVP as the conditioning and stabilizing agent, respectively. During the nucleation of MIL-53(Fe), the PVP droplet, as a nano-reactor, controlled the growth of the crystal nucleus. The size and aspect ratio (length/width) of nanocrystals increased with an increase in PVP in the synthetic mixture. The MIL-53(Fe) nanocrystals showed a homogeneous morphology, with approximately 190 nm in length and 100 nm in width. MIL-53(Fe) not only was used to load the anticancer drug doxorubicin (DOX) but also generated hydroxyl radicals (˙OH) via a Fenton-like reaction for ROS-mediated/chemo-therapy of cancer cells. The approach was expected to synthesize numerous types of nano-size iron(III)-based MOFs, such as MIL-53, 89, 88A, 88B and 101. The MIL-53(Fe) nanocrystals hold great promise as a candidate to improve the controlled release of drugs and treatment effect for cancer therapy.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 17
·8334-8346
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IF 3.3
Peifu Sun,Xiao Zhang,Zhiren Guo,Xinyue Liu,Yuanming Lan,Dongxiang Zhang,Hansheng Li,Jinying Li,Helei Liu,Xiyan Xu
The excessive discharge of isothiazolinone bacteriostatic agent-containing wastewater has posed serious threats to human health and environmental safety. As 1,2-benzisothiazolin-3-one (BIT) is one of the most commonly used isothiazolinones, its effective degradation is necessary and urgent. In the current study, a NH2-MIL-53(Fe)-based adsorptive photo-Fenton-like system was constructed for efficiently adsorbing and photodegrading BIT under solar light. The equilibrium BIT adsorption capacity Qe of NH2-MIL-53(Fe) reached 1140.89 mg g−1. The adsorptive photo-Fenton-like system has achieved more than 90% removal of BIT using NH2-MIL-53(Fe) in the presence of H2O2 under solar light irradiation, and the band gap of NH2-MIL-53(Fe) was calculated by UV-Vis analysis to be 2.10 eV. The influences of pH, dosage of photocatalysts and H2O2 were also assessed. It was found that H2O2 reduced the recombination of electron–hole pairs, and the radical quenching experiments and EPR testing result confirmed that h+, ˙OH and O2˙− played a crucial role in the photocatalytic process. This study supports the application of Fe-based MOF materials for simultaneous adsorption and the solar light photocatalytic degradation of BIT.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2016
·
IF 8.328
Yaowen Gao,Simiao Li,Yixi Li,Linyu Yao,Hui Zhang
Photocatalysis based on metal-organic frameworks (MOFs) is being actively investigated as a potential technology in visible light harvesting and utilizing processes. Herein we report that MIL-53(Fe), an earth-abundant Fe-containing MOF material, shows photocatalytic activity for the degradation of Acid Orange 7 (AO7) from aqueous solution under visible LED light irradiation, yet the photocatalytic performance of bare MIL-53(Fe) was not satisfactory due to the fast recombination of photoinduced electron-hole pairs. This can be effectively overcome by adding the external electron acceptor (e.g., persulfate, PS) to the catalytic process. The accelerated photocatalytic degradation of AO7 is demonstrated by the result that the degradation efficiency of AO7 in the MIL-53(Fe)/PS/Vis process reached almost 100% within 90 min as compared to only 24% under the identical experimental conditions for the MIL-53(Fe)/Vis process. To investigate the mechanism of the MIL-53(Fe)/PS/Vis process, photoluminescence (PL) spectra, electrochemical measurements and electron paramagnetic resonance (EPR) analysis were performed. It was concluded that the efficient separation of photogenerated electrons and holes by the introduced PS and the subsequent formation of reactive radicals resulting from the activation of PS by photogenerated electrons accounted for the accelerated photocatalytic degradation of AO7 in the MIL-53(Fe)/PS/Vis process. Furthermore, the applicability of MIL-53(Fe) used in the persulfate-mediated photocatalytic process was systematically investigated in terms of the identification of reactive radicals, the reusability and stability of the photocatalyst, as well as the effect of operating parameters. The findings of this work highlighted the great potential of MOFs as photocatalysts and elucidated a new opportunity for persulfate remediation of contaminated water.
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JOURNAL OF HAZARDOUS MATERIALS
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2015
·
IF 4.529
Ruowen Liang,Fenfen Jing,Lijuan Shen,Na Qin,Ling Wu
A bifunctional photocatalyst-Fe-benzenedicarboxylate (MIL-53(Fe)) has been synthesized successfully via a facile solvothermal method. The resulting MIL-53(Fe) photocatalyst exhibited an excellent visible light ( λ ≥ 420 nm) photocatalytic activity for the reduction of Cr(VI), the reduction rate have reached about 100% after 40 min of visible light irradiation, which has been more efficient than that of N-doped TiO 2 (85%) under identical experimental conditions. Further experimental results have revealed that the photocatalytic activity of MIL-53(Fe) for the reduction of Cr(VI) can be drastically affected by the pH value of the reaction solution, the hole scavenger and atmosphere. Moreover, MIL-53(Fe) has exhibited considerable photocatalytic activity in the mixed systems (Cr(VI)/dyes). After 6 h of visible light illumination, the reduction ratio of Cr(VI) and the degradation ratio of dyes have been exceed 60% and 80%, respectively. More significantly, the synergistic effect can also be found during the process of photocatalytic treatment of Cr(VI) contained wastewater under the same photocatalytic reaction conditions, which makes it a potential candidate for environmental restoration. Finally, a possible reaction mechanism has also been investigated in detail.
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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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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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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Ying Jiang,Hao Lu,Lingli Lei,Daniel Scherman,Yingshuai Liu
The design of nanomedicines targeting specific tumor microenvironment (TME) characteristics, such as low pH, hypoxia, and elevated glutathione (GSH) concentration, holds significant potential for selectively killing cancer cells. In this study, we have developed a TME-responsive nanoparticle, i.e. , MIL-53(Fe)@MnO 2 stabilized with polyethylene glycol (FMP), which is capable of depleting GSH and sustainably generating hydroxyl radical (•OH) for enhanced chemodynamic therapy of cancer. After endocytosis, the FMP nanoparticles undergo gradual decomposition, resulting in GSH depletion while releasing Fenton-active Fe 2+ and Mn 2+ ions. These ions then subsequently catalyze a Fenton-like reaction to generate highly toxic •OH, ultimately inducing oxidative cell death. As a synergistic effect, the depletion of GSH further enhances therapeutic efficacy by inhibiting intracellular •OH scavenging. In vivo experiments demonstrated that this synergistically chemotherapeutic approach efficiently suppressed tumor growth without inducing significant systemic toxicity. This work presents a promising nanotherapeutic strategy that simultaneously depletes intracellular GSH and sustains cytotoxic •OH generation for enhanced tumor treatment.
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Journal of Water Process Engineering
·
2025
·
IF 6.7
Jincheng Dai,Shuyue He,Xiyu Song,Chuliang Shen,Hongjuan Zhang,Ruyi Xie
The application of Fe-based metal-organic frameworks in photo-Fenton antibiotic degradation is limited by the low charge separation efficiency and slow Fe 3+ /Fe 2+ transition. In this study, a novel Z -scheme porous carbon nitride/mixed-valent MIL-53(Fe) (KCM-20) heterojunction photocatalyst was successfully constructed for degradation of high concentration tetracycline. On the one hand, the Z -scheme heterojunctions system is conducive to the rapid separation of photogenerated electron-hole pairs. On the other hand, the cyclic conversion of Fe 3+ /Fe 2+ in the MIL-53(Fe) photo-Fenton system can be accelerated. The KCM-20 showed the highest degradation efficiency for tetracycline. The KCM-20/light/H 2 O 2 system degraded more than 93 % of tetracycline (150 mg·L −1 ) within 75 min and exhibited the highest degradation kinetic constant, which is 8.0 and 2.4 times higher than those of carbon nitride and MIL-53(Fe), respectively. Its excellent catalytic performance can be attributed to the efficient synergy between photocatalytic reaction and Fenton reaction, producing more active species for tetracycline degradation. EPR and activity capture experiments indicate that ·O− 2, ·OH and h + are the main active species for tetracycline degradation. By analyzing the intermediate products, three degradation pathways for tetracycline were proposed. This work provides a new pathway for the preparation of efficient and cost-effective photocatalysts for the degradation of organic pollutants.
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Journal of Environmental Chemical Engineering
·
2024
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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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2019
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IF 5.107
Yuqi Cui,Li-chao Nengzi,Jianfeng Gou,Yan Huang,Bo Li,Xiuwen Cheng
Z-scheme heterojunction photocatalyst can simultaneously reduce the recombination of photo-generated electron-hole pairs and preserve its outstanding redox ability during the process of photocatalytic reaction. In this study, Z-scheme MIL-53(Fe)/α-Bi 2 O 3 /g-C 3 N 4 photocatalyst was successfully fabricated via an accessible method and comprehensive characterized by XRD, FT-IR, SEM, TEM, XPS, N 2 adsorption-desorption isotherms, UV–vis diffuse reflection spectroscopy and photoelectrochemical analysis. The as-obtained MIL-53(Fe)/α-Bi 2 O 3 /g-C 3 N 4 composite exhibited superior photocatalytic activity for amino black 10B degradation than that of pure g-C 3 N 4 , α-Bi 2 O 3 , MIL-53(Fe) and α-Bi 2 O 3 /g-C 3 N 4 binary composite under visible light irradiation and the photodegradation rate would achieve the maximum when the mass fraction of MIL-53(Fe) was 32% in ternary composite. The enhanced photocatalytic performance of MIL-53(Fe)/α-Bi 2 O 3 /g-C 3 N 4 ternary composite could be mainly ascribed to improved visible light absorption range and the construction of an effective interfacial heterojunction driven by direct solid-state dual Z-scheme mechanism, which significantly facilitates the separation and transfer of photo-generated charge carriers. Eventually, the as-prepared ternary composite was confirmed to have prominent stability and reusability after consecutive 4 recycling run.
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Water
·
2025
·Vol. 17
·期 9
·1309
·
IF 3
Xiaoyan Ma,Rongbin Quan,Wenqing Cao,Weijie Zhang,Su Jiang,Jiao Feng,Jiulong Wang,Stefanos Giannakis
Electrochemical reduction is a promising strategy for the dechlorination of halogenated organic compounds, offering advantages such as enhanced electron transfer efficiency and increased hydrogen atom concentration. It has garnered significant attention for application in mitigating halogenated disinfection by-products (DBPs) in drinking water, owing to its high efficiency and simple operation. In this study, trichloroacetic acid (TCAA), a representative DBP, was selected as the target contaminant. A novel composite cathode comprising a metal–organic framework MIL-53(Fe)@C supported on an Nd magnet (MIL-53(Fe)@C-MAG) and its dechlorination performance for TCAA were systematically investigated. The innovative aspect of this study is the magnetic attachment of the MOF catalyst to the carbonized cathode surface treated through carbonization, which fundamentally differs from conventional solvent-based adhesion methods. Compared to the bare electrode, the MIL-53(Fe)@C-MAG achieved a TCAA removal efficiency exceeding 96.03% within 8 h of contact time. The structural characterization revealed that the α-Fe0crystalline phase serves as the primary active center within the MIL-53(Fe)@C catalyst, facilitating efficient electron transfer and TCAA degradation. The scavenger experiments revealed that TCAA reduction involves a dual pathway: direct electron transfer and atomic hydrogen generation. The modified MIL-53(Fe)@C-MAG electrode exhibited robust electrolytic performance over a broad pH range of 3–7, with TCAA removal efficiency showing a positive correlation with current density within the range of 10–50 mA/cm2. Furthermore, the electrode maintained exceptional stability, retaining more than 90% removal efficiency after five consecutive operational cycles. The versatility of the system was further validated by the rapid and efficient dechlorination of various chlorinated DBPs, demonstrating the broad applicability of the electrode. The innovative magnetic composite electrode demonstrates a significant advancement in electrochemical dechlorination technology, offering a reliable and efficient solution for the purification of drinking water contaminated with diverse halogenated DBPs. These results provide valuable insights into the development of electrolysis for dechlorination in water treatment applications.
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Sustainable Materials and Technologies
·
2025
·
IF 9.2
Xianjin Qi,Guizhi Yan,Boyu Du,Mengmeng Wang,Yongkui Li
Arsenic (As) contamination is a global problem that requires innovative remediation, this study successfully synthesized a novel MnFe 2 O 4 -Zn/Co ZIFs@MIL-53(Fe) (MFZM) using a solvent method to remove As(V) from contaminated water. The MFZM exhibited a rhomboidal dodecahedron structure with a high specific surface area of 158.93 m 2 /g, which contributed to its exceptional adsorption performance under both acidic and neutral pH conditions. Notably, the adsorption capacity for As(V) reached approximately 599.90 mg/g at an equilibrium concentration of 500 mg/L, surpassing the performance of several previously reported adsorbents. The kinetic modelling results indicated that the adsorption process followed a pseudo-second-order mechanism, suggesting chemisorption as the dominant process. However, the isotherm studies demonstrate favorable single-layer adsorption, with the Langmuir model providing the best fit for the experimental data. The X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy with energy-dispersive spectroscopy (SEM-EDS) analysis revealed that the Fe/Mn/Co on the MFZM surface can hydrolyze and generate Fe/Mn/Co-OH groups under pH conditions ranging from 3 to 7, facilitating the formation of stable coordination complexes with As(V). Furthermore, the MFZM provided abundant positively charged adsorption sites that effectively attracted HAsO 4 2− via electrostatic interactions, leading to efficient As(V) removal. These findings underscore the potential of the MFZM as a promising adsorbent for the effective remediation of As-contaminated wastewater, supporting sustainable environmental management.
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