WATER AIR AND SOIL POLLUTION
·
2024
·Vol. 235
·期 5
·1-17
·
IF 3.8
Zhou Zhuyou,Ji Yufeng,Wang Yong,Liu Menghe,Xu Ying,Liu Ruijie,Yang Mingjie,Zou Congyang
In this study, the carbon-doped bimetallic organic framework C 60 /MIL-101(Fe,Cu) catalyst was prepared for the first time via solvothermal synthesis method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), and a series of other instruments. At the same time, methylene blue (MB) was used as the target degradation material to investigate the catalytic performance of H 2 O 2 for MB degradation under visible light. The degradation experiment showed that the removal rate of C 60 /MIL-101(Fe,Cu) to MB reached 99.2% within 80 min. Furthermore, cyclic experiments demonstrated good stability and reusability of the catalyst. Finally, the degradation mechanism of the reaction was deduced by quenching experiment, UV–vis diffuse reflection and mott-Schottky plots. The results show that hydroxyl radical (·OH) and superoxide radical (·O 2 − ) play a major role in the degradation of MB during photo-Fenton process.
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INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Shen Zhang,Yaxian Qiao,Shiwei Luo,Bingbing He,Jingliang Xu
We reported a bifunctional site-isolated Lewis acid-Brønsted base metal-organic frameworks (NH 2 -Mo-MIL-101(Al)) for selective epimerization and isomerization of glucose to mannose and fructose. The yields of mannose and fructose were 34.09 % and 19.25 %, respectively, at 120 °C for 40 min. The sum selectivity of mannose and fructose was 95.64 %. System characterization showed that the excellent catalytic performance may attribute to the synergistic effect of Lewis acid (MoO 2 and MoO 3 ) sites and Brønsted base (-NH 2 ) sites on NH 2 -Mo-MIL-101(Al). The composition of the catalyst before and after catalysis experiment was characterized by ICP-MS. Results showed that no Mo specie was leached from NH 2 -Mo-MIL-101(Al) after 5 times re-used. 97 % of catalytic efficiency was retained after 5 times reusing compared to origin NH 2 -Mo-MIL-101(Al). The N-Mo chemical bonding between Mo active sites with NH 2 -MIL-101(Al) skeleton enhanced the hydro-stability and hydrothermal cyclic stability. Notably, 94.13 % of total sugar recovery was achieved from reaction solution by sample crystallization process without requiring chromatographic separation. High purity of glucose (91.27 %) and mannose (88.53 %) were recovered from reaction solution. This study provided a green and feasible catalytic and recovery process for industrial production of high-yield mannose and fructose from glucose.
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LANGMUIR
·
2025
·
IF 3.9
Yue Cao,Yanping Wang,Lirong Guo,Zhiyue Han,Haining Liu,Kaipeng Zhong,Shaoju Bian,Naicai Xu
A novel composite adsorbent, AMP@MIL-101(Cr), has been successfully synthesized by integrating ammonium phosphomolybdate (AMP) with the metal–organic framework MIL-101(Cr) for the efficient adsorption of rubidium ions (Rb+) from aqueous solutions. The results of structural characterizations confirmed that the crystalline framework of the adsorbent remained intact after Rb+ adsorption, indicating excellent structural stability. Adsorption kinetics, isotherm, and thermodynamics studies revealed that the adsorption process followed a single-layer chemisorption mechanism and was an endothermic reaction and spontaneous adsorption process with negligible influence from solution pH. The adsorbent exhibited a remarkable Rb+ adsorption capacity, reaching 69.4 mg·g–1 within 5 min in a solution containing 250 mg·L–1 Rb+ at 45 °C. In the Nanyi Mountain Oilfield, the adsorption rate of adsorbent for Rb+ (10.69%) exceeded that of other ions (Li+: 0.75%; Na+: 0; K+: 0.95%; Mg2+: 0.67%). Furthermore, the adsorbent still maintained 86.72% of its initial adsorption capacity after 5 consecutive adsorption–desorption cycles. These findings highlighted the great potential of AMP@MIL-101(Cr) as an efficient and stable adsorbent for the selective recovery of rubidium from aqueous environments.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 8
·2864-2872
·
IF 6.119
Xiaoli Li,Yuan Tang,Yue Jiang,Manman Mu,Xiaohong Yin
A series of composites composed of Bi4O5Br2 and Fe-MIL were successfully fabricated for mimicking sunlight-driven photocatalytic reduction of CO2. Herein, Bi4O5Br2, as a modulator of solid acids, could turn NH2-MIL-101(Fe) into NH2-MIL-88B(Fe) completely at 0.07 wt% catalytic loading, where further addition could construct the corresponding composites of Bi4O5Br2 and NH2-MIL-88B(Fe). The highest activity in the photocatalytic reduction of CO2 was achieved at 7.96 μmol g−1 h−1 of CH4 at 3.28 wt% of Bi4O5Br2. Besides, this catalyst possessed high photostability during the recycling experiments and the mechanism of this process was thoroughly explored. This study provides a novel strategy employing solid acid modulators for regulating the structure and morphology of MOFs showing high activity and stability in the photocatalytic reduction of CO2 to CH4.
研究领域:
材料科学
·
环境科学
·
化学
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Materials Today Chemistry
·
2026
·
IF 7.4
Yu Xia,Aiping Wang,Qiao Hu,Guangming Han,Kaidi Gao,Yangyang Gao,Ruize Wang,Yongqi Wang,Jianfeng Yao
A well-designed Fe-N dual sites amino-functionalized (MIL-101(Fe)-NH 2 ) separator is fabricated. • The unsaturated Fe sites in the MOF act as strong anionphilic modifiers to adsorb PF 6 − . • The polar -NH 2 groups act as Lewis's base sites to enhance electrolyte wettability. • The synergistic Fe-N sites induce the formation of a stable solid electrolyte interphase. • This separator can regulate lithium deposition and enable high-performance lithium metal batteries. Lithium-based batteries utilizing metallic lithium anodes have attracted widespread research interest due to their exceptional theoretical energy density. However, the growth of dendritic lithium structures, unstable solid electrolyte interphase (SEI) and associated safety concerns pose substantial obstacles to their commercial application. Traditional polypropylene (PP) separators suffer from poor electrolyte affinity and electrochemical inertness, causing heterogeneous Li + distribution and severe interfacial polarization. Herein, an amino-functionalized MIL-101(Fe)-modified PP separator is successfully developed to regulate Li deposition through the synergistic effects of Fe-N dual active sites. The unsaturated Fe sites in the MOF act as strong anionphilic modifiers to adsorb PF 6 − and suppress anion migration; the polar -NH 2 groups act as Lewis's base sites to enhance electrolyte wettability and accelerate ion transport. These synergistic Fe-N sites induce the in-situ formation of a stable LiF/Li 3 N-rich and flexible inorganic-organic hybrid SEI, preventing the penetration of dendritic lithium. Electrochemical testing reveals that the Li|Li symmetric cells achieve more than 650 h of uniform lithium deposition and also stable cycling at elevated temperatures. Furthermore, the LiFePO 4 |Li cells and the LiFe 0.5 Mn 0.5 PO 4 |Li cells employing this modified separator demonstrate superior cycling stability and enhanced rate capability. Modifying separators with functionalized metal-organic frameworks (MOFs) presents a plausible strategy to improve the performance of electrochemical batteries, contributing to an in-depth discussion of the application of MOFs in lithium battery technology. Amino-functionalized separators (PP@MIL-101-NH 2 ) are successfully designed to regulate ion transport for high-performance lithium metal batteries. The unsaturated Fe sites in the MOF act as strong anionphilic modifiers to adsorb PF 6 − ; the polar -NH 2 groups act as Lewis's base sites to enhance electrolyte wettability. Synergistic Fe-N sites induce the formation of a stable LiF/Li 3 N-rich solid electrolyte interphase, preventing the penetration of dendritic lithium. Download: Download high-res image (365KB) Download: Download full-size image
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Applied Materials Today
·
2026
·
IF 7
Madiha Rafiq,Dan Liao,Changkun Liu
Ternary g-C 3 N 4 /Ti 3 C 2 T x /MIL-101(Fe) photocatalyst was constructed via in situ assembly. • Ti 3 C 2 T x promotes interfacial charge separation and accelerates electron transfer. • Rapid in situ H 2 O 2 generation enables an oxidant-free visible-light photo-Fenton process. • CTF achieves efficient, broad-spectrum degradation of dyes and PPCPs. Visible-light photo-Fenton oxidation represents a promising strategy for removing dyes and pharmaceuticals/personal care products (PPCPs), which are persistent water contaminants. However, its broader application is constrained by challenges such as inefficient charge separation and dependence on externally added hydrogen peroxide (H 2 O 2 ). In this study, a ternary g-C 3 N 4 /Ti 3 C 2 T x /MIL-101(Fe) photocatalyst was synthesized via the in-situ growth of MIL-101(Fe) on g-C 3 N 4 /Ti 3 C 2 T x , enabling efficient visible-light-driven, zero-external H 2 O 2 -added photo-Fenton degradation of organic pollutants. The hybrid system exhibits significantly enhanced oxygen activation and interfacial electron-transfer capability, with in situ H 2 O 2 generation rates about three times higher than those of pristine g-C 3 N 4 . Under visible-light irradiation, the composite continuously produces reactive oxygen species ( ∙ O 2 - , and ∙ OH) at substantially higher levels than g-C 3 N 4 and g-C 3 N 4 /MIL-101(Fe), indicating promoted charge separation and faster interfacial electron transfer. As a result, the catalyst enables broad-spectrum pollutant removal within 60 min, achieving degradation efficiencies of 99.78% (methylene blue), 99.49% (rhodamine B), 88.27% (tribromophenol), 61.50% (doxycycline hydrochloride), and 78.98% (levofloxacin). Overall, rapid in situ H 2 O 2 formation, coupled with efficient ROS generation, enables high-performance pollutant degradation without the need for external oxidant dosing, providing a green strategy for degrading dyes and PPCPs under visible light. Download: Download high-res image (174KB) Download: Download full-size image A ternary g-C 3 N 4 /Ti 3 C 2 T x /MIL-101(Fe) photocatalyst enables visible-light-driven, oxidant-free photo-Fenton degradation of dyes and PPCPs through MXene-promoted charge separation and rapid in situ H 2 O 2 generation. The self-generated H 2 O 2 activates Fe 3+ /Fe 2+ cycling to continuously produce h + , ∙O 2 - , and ∙OH, achieving efficient pollutant mineralization.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2026
·
IF 9.1
Xinchun Liu,Ruyu Zhao,Xiaolin Li,Daidai Wang,Yinyong Sun
A novel and robust catalyst for oxidative desulfurization (ODS) of fuel oil was fabricated by encapsulating titanium-oxo clusters with amino-groups (Ti 6 abz 6 , abz denotes 4-aminobenzoic acid) into the mesoporous cages of MIL-101(Cr). This strategy employs an amidation reaction with succinic anhydride that acts as a molecular expander to realize an expansion-trapping process. This approach can effectively prevent clusters aggregation/leaching while maintaining the accessibility of active sites. The optimized catalyst named as 0.4Ti 6 abz 6 @MIL exhibited superior catalytic performance in the ODS reaction of DBT. Its turnover frequency reached 61.3 h −1 at 60 °C, which is much higher than those of the composites prepared by impregnation and physical-mixing methods. The results from electron paramagnetic resonance indicate that hydroxyl radicals (•OH) are the dominant active species in the oxidation reaction. Furthermore, density functional theory calculations revealed that the introduction of amide linkages significantly strengthens the adsorption of H 2 O 2 through enhanced hydrogen-bonding interactions, inducing the elongation of peroxoxide bond and effectively facilitating its cleavage to generate reactive •OH radicals. This work demonstrates that amidation is an effective strategy for encapsulating highly dispersed and stable titanium-oxo clusters into the pores of MOFs.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 30
·1-21
·
IF 2.8
Yang Minjie,Zou Congyang,Ji Yufeng,Liu Ruijie,Xu Ying
A novel MIL-101(Fe)/Bi₂S₃ Z-scheme heterojunction with a metal–organic framework (MOF) structure was synthesized via a solvothermal method. Compared with pristine MIL-101(Fe) and pristine Bi₂S₃, this composite exhibits a significant breakthrough in degradation performance toward rhodamine B (RhB) and tetracycline hydrochloride (TCH). Specifically, it achieves a degradation efficiency of 95.7% for 20 mg/L TCH within 120 min and 98.6% for 40 mg/L RhB within 90 min.Characterizations including X-ray diffraction (XRD), scanning electron microscopy (SEM), ultraviolet–visible diffuse reflectance spectroscopy (UV–Vis DRS), and electrochemical impedance spectroscopy (EIS) confirm that the MOF structure of MIL-101(Fe) provides a stable support matrix for Bi₂S₃. Moreover, the construction of the Z-scheme heterojunction can effectively suppress the recombination of photogenerated electron–hole pairs while retaining the strongly oxidizing hydroxyl radicals (・OH) and strongly reducing superoxide radicals (・O₂⁻). More importantly, after five recycling cycles, the degradation efficiencies of the composite for TCH and RhB remain at 86.8% and 88.6%, respectively, with no obvious damage to its crystal structure after cycling. This demonstrates superior structural stability and reusability compared to most reported MOF-based photo-Fenton catalysts.
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CELLULOSE
·
2022
·Vol. 30
·期 2
·1171-1191
·
IF 6.123
Tu Chao,Sun Zenghui,Huang Fei,Wu Ziwei,Chen Hang
The photocatalytic process is an energy-saving and high-efficiency wastewater treatment technology. In this work, a simple in-situ hydrothermal method was used to prepare a photocatalytic material based on waste loofah with high efficiency, reusability and excellent heterostructure to improve the photodegradation efficiency. The prepared MoS 2 @MIL-101(Fe)@Carboxylated loofah composite material was characterized by scanning electron microscope (SEM), electrochemical impedance spectroscopy (EIS), UV–Vis diffuse reflection spectroscopy (UV–vis DRS), X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and transient photocurrent (TPC). The composite material demonstrated high adsorption capacity for hydrochloride (TC) and methylene blue (MB) and photocatalytic capacity under visible-light irradiation at room temperature which were attributed to the porous structure, strong visible-light absorption, and low recombination velocity of electron–hole pairs due to the heterojunctions. The loofah sponge used as a substrate can provide a means for powder catalyst recovery and waste cellulose recycling. Meanwhile, the photocatalyst proved excellent stability in the MB degradation experiment and could be reused for four cycles.
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ACS Omega
·
2023
·
IF 4.1
Qiyue Zhang,Aori Qileng,Jiale Li,Yiran Cao,Weipeng Liu,Yingju Liu
Organic dyes can produce harmful effects on the water environment, such as affecting the growth of aquatic organisms, reducing the transparency of water bodies, and causing eutrophication of water bodies, so it is necessary to mitigate the hazards of organic dyes. In this study, a metal–organic framework [NH2-MIL-101(Fe)] was synthesized by the solvothermal method as a carrier for the in situ uniform deposition of AgCl nanoparticles on its surface, which was successfully used for both adsorption and degradation of Congo red. Adsorption results showed that the adsorption kinetics conformed to the proposed secondary adsorption kinetics equation with a maximum adsorption capacity of 248.4 mg·g–1. Furthermore, the degradation results indicated that with the aid of sodium borohydride as a reducing agent, the degradation of Congo red followed pseudo-first-order kinetics with a degradation rate of 0.077 min–1, and the complete degradation of Congo red was finished within 18 min. Therefore, AgCl/NH2-MIL-101(Fe) may find a potential application in the removal of dyes from wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Peipei Huang,Qing Chang,Guodong Jiang,Keru Xiao,Xu Wang
Metal organic frameworks are important Fenton-like materials in environment remediation. Nevertheless, the slow Fe(III)/Fe(II) cycling and low H 2 O 2 utilization limit their application. In this study, we develop the ferrous bimetallic MIL-101(Fe II 3 , Mn), which significantly enhanced catalytic performance (5.8 and 31.4-fold higher phenol removal rate and apparent rate constant, respectively) compared with the original MIL-101(Fe). The mechanisms are fully investigated by XPS, EPR and DFT. The Fe 2+ substitution affords the mixed-valences of Fe(III)/Fe(II) in the frameworks, which serve as stronger sites for H 2 O 2 activation. Mn in MIL-101(Fe II 3 , Mn) can also function as another reaction center to activate H 2 O 2 . Catalysts could coordinate with the π–electrons of pollutants, resulting in the electron transfer from pollutants to MIL-101(Fe II 3 , Mn). Moreover, electrons around Mn atoms tends to transfer to the region of Fe atoms owing to the electronegativity difference, inducing to strengthen the electron-rich Fe micro-region. Therefore, H 2 O 2 was primarily adsorbed onto electron-rich regions where it would be efficiently reduced to •OH, contributing to a higher H 2 O 2 utilization (81.2 %). This study opens new insight into design of Fe-based MOFs as highly efficient Fenton-like catalysts in wastewater treatment.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Ziyi Xiao,Rui Wu,Tingting Shu,Yingxi Wang,Ling Li
In order to further improve the catalytic performance of MIL-101, cobalt-doped MIL-101(Fe,Co) was synthesized by solvothermal method. By adjusting the ratio of cobalt doping, the MIL-101(Fe,Co 20% ) with the best catalytic activity was obtained. The activation performance of MIL-101(Fe,Co 20% ) for peroxymonosulfate (PMS) was studied using Rhodamine B (RhB) as a pollutant model. The experimental results proved MIL-101(Fe,Co 20% ) with much better catalytic performance than MIL-101(Fe), which can degrade more than 99% of RhB within 15 min. The effects of initial solution pH and coexisting anions in water on the degradation of RhB were further discussed. The results showed that MIL-101(Fe,Co 20% ) was with excellent stability and degradation efficiency can still keep above 90% after five cycles. The free radical quenching experiments were further studied to explore the degradation mechanism. It can be concluded that SO 4 - · was the main active free radical for the degradation of RhB. The possible intermediate products in the degradation process of RhB were analyzed by LC-MS. Combined with the comparison of XPS before and after the reaction, the possible reaction mechanism of RhB degradation process was inferred.
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