Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Jiepeng Zhao,Yifei Ma,Zhaomin Tong,Mei Wang,Liantuan Xiao,Suotang Jia,Xuyuan Chen
Engineering photocatalyst crystal facets and constructing heterojunctions are effective strategies to improve photocatalytic activity. The amino-modified titanium-based metal–organic framework (MOF) NH 2 -MIL-125(Ti) (NM) has drawn extensive attention as a photocatalyst by virtue of its high specific surface area, abundant pore structure, and narrow bandgap. However, its catalytic activity is hindered by fast electron-hole recombination and limited light absorption. This study synthesizes NM with engineered crystal facets and Co 3 O 4 @NH 2 -MIL-125(Ti) (C-NM) composites with varying Co 3 O 4 loadings using a facile hydrothermal method. The impact of heterojunctions and facet design on photocatalytic CO 2 reduction under visible light is also studied. Results show that the C-NM, with exposed {111} facets and optimal Co 3 O 4 loading, demonstrates superior photocatalytic CO and CH 4 production rates of 21.64 μmol h −1 g −1 and 3.99 μmol h −1 g −1 , 2.1 and 1.6 times higher than those of NM {001} , respectively. Experimental characterization and density functional theory (DFT) analyses attribute the improved photocatalytic activity to several mechanisms. First, crystal facet modulation can optimize the active sites and specific surface area of the photocatalysts. Second, by loading the narrow-bandgap Co 3 O 4 nanoparticles, bandgap of the C-NM photocatalyst is further reduced, thereby enhancing the absorption and utilization of visible light. Finally, the NM/Co 3 O 4 heterostructure minimizes electron-hole recombination, significantly boosting CO 2 reduction efficiency.
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OPTICAL MATERIALS
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2024
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IF 3.8
Yixuan Liu,Jiamin Wei,Qi Zong,Chaoyue Chen,Tinghai Yang,Weiqiao Liu
Constructing cost-efficient and robust Fe-MIL-based photocatalysts for efficiently photodegrading antibiotics is highly appealing, however, their intrinsic defects, particularly unsatisfied visible light harvesting efficiency and rapid recombination of charge carriers, provide significant challenges. Herein, oxygen-vacancy-rich Bi 2 WO 6 -OVs/NH 2 -MIL-88B (Fe) composites were successfully constructed via a two-step approach consisting of a hydrothermal reaction followed by NaBH 4 treatment. The chemical compositions, microstructure, morphology, as well as optical properties of the as-prepared samples were thoroughly established. The optimized Bi 2 WO 6 -OV(40)/NH 2 -MIL-88B(Fe) photocatalyst exhibited the maximum photocatalytic efficiency (95.3 %) for the photodegradation of Norfloxacin (NOR), which was considerably greater than that of the heterostructure (56.9 %). The enhancement of photocatalytic performance can be attributed to the collaborative effect between oxygen vacancies and hybrid heterojunctions, which jointly enhances photoexcited electron generation and accelerates charge transfer. Furthermore, from the perspective of practical applications, the effects of pH, NOR concentration, and photocatalyst reuse were carefully investigated. The radical trapping experiments and ESR results verified that superoxide radicals (•O 2 − ), holes (h + ), and hydroxyl radicals (•OH) were the main active species in the NOR degradation process, and the possible photocatalytic mechanism was speculated accordingly. This research provides a promising approach to fabricating Fe-MOF-based heterojunctions with surface oxygen vacancy defect modification for the photodegradation of antibiotics.
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LANGMUIR
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2025
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IF 3.9
Guang Lu,Lunqiu Zhang,Jiling Liang,Wei Li,Zheng Li,Xuejun Zou,Xiaodong Zhang
Herein, first, MIL-125 samples were synthesized via a hydrothermal method. Then, Ag species were doping on the surface of MIL-125 samples via the photolysis of silver nitrate. Finally, the Z-scheme MIL-125/Ag/BiOBr composite was synthesized via a directed liquid assembly method. The structure, morphology, and optical properties of the prepared samples were investigated via X-ray diffraction, scanning electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopic mapping, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, N2 adsorption–desorption analysis, ultraviolet–visible spectroscopy, photoluminescence spectroscopy, surface photovoltage analysis, transient photocurrent response analysis, electrochemical impedance spectroscopy, and electron spin resonance analysis. Photocatalytic experiments indicated that the photocatalytic Cr6+ reduction efficiency of MIL-125/Ag/BiOBr heterojunctions was 85.7% at pH = 6, which was approximately 5.5 and 2.2 times higher than that using BiOBr and MIL-125 alone, respectively. This performance was attributed to the intimate interfacial contact between MIL-125 and BiOBr and the doping of Ag species, which increased the transfer and separation of photogenerated carriers and inhibited the recombination of electrons and holes. Furthermore, the possible photocatalytic Cr6+ reduction mechanism of the Z-scheme MIL-125/Ag/BiOBr photocatalyst was proposed.
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INORGANIC CHEMISTRY
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2024
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IF 4.3
Yuhao Che,Wenhui Li,Chunqi Wang,Xuemin Zhang,Zilei Guo,Aziz Bakhtiyarovich Ibragimov,Junkuo Gao
The development of materials with superior thermal insulation and flame retardancy is critical for industrial applications and daily life. Metal–organic framework (MOF)@poly(vinyl alcohol) (PVA) (MOF@PVA) aerogel composites have demonstrated remarkable thermal insulation and flame retardancy properties. In this work, MIL-53(Al) was directly mixed with PVA and formed by freeze-drying, and the influence of the pore structure on the thermal insulation and flame retardancy properties of the materials was investigated. The incorporated MIL-53(Al) nanoparticles introduced abundant micro- and mesopores, enhancing the complexity of the pore structure and improving the thermal insulation and flame retardancy properties of the aerogels. The directionally freeze-cast aerogel achieved a thermal conductivity of 0.040 W·mK–1, and maintained excellent thermal insulation ability even at 220 °C. Furthermore, the aerogel exhibited nonflammable and self-extinguishing characteristics. This environmentally friendly manufacturing method provides new ideas for the design of MOF-based composites, thereby expanding their application areas.
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Yao Ji,Zhiyuan Pan,Tiangang Ma,Ke Wang,Xiaoxian Zhao,Quan Jin
Hierarchical porous spindle-shaped MIL-88B (HPS-MIL-88B) with core-shelled structure was prepared by citric acid-assisted. The material exhibits open channels on its outer surface and a hierarchical internal cavity structure with meso-/macro-pores. The samples were then pretreated at 200 °C to form an oxide film , aiming to improve the conductivity of material. The as-prepared HPS-MIL-88B-6 h@Fe 2 O 3 material with core-shelled structure exhibits superior selectivity and high sensitivity to trimethylamine (TMA) at 200 °C (detection limit as low as 1 ppm) with fast response and excellent repeatability. The outstanding sensing performance was owing to the open and hierarchical porous that enhances the reaction between the target gas and the active sites of the material. In addition, the metal unsaturated active sites of MIL-88B (Lewis’s acid) can selectively undergo acid-base reactions with TMA (Lewis’s base), enhancing the generation of oxygen species and improving the selective adsorption capacity towards the target gas. This work provides a new path route for the application of MOF materials in sensors.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yong Fu,Pengyi Zhang,Xianjie Wang
We developed a feasible strategy to obtain the defective MIL-100(Cr) (De-M) via doping 3,5-pyridinedicarboxylate and subsequently loaded polydivinylbenzene (PDVB) by thermal deposition to obtain a hydrophobic MOFs composite (De-M@PDVB). De-M 10 (10 % defective ligand/total ligands) exhibited excellent performance for the capture of toluene due to uniform particle size, high specific surface area and pore volume. Subsequent thermal deposition with PDVB further increased the hydrophobicity, as-obtained De-M 10 @PDVB in the dynamic adsorption experiment showed about 2 and 1.5 time adsorption capacity as that of primary MIL-100(Cr) and De-M 10 under 50 % RH at 298 K. In addition, the toluene uptake of De-M 10 @PDVB (0.95, 298 K) in static adsorption experiments was 1320 mg/g, much higher than many reported MOFs. Furthermore, De-M 10 @PDVB could be regenerated at 378 K, demonstrating its excellent regenerability at low temperature. The adsorption mechanism of toluene on De-M 10 @PDVB could be attribute to the π-π stacking interaction between the benzene ring of toluene with H 3 BTC and adsorption sites offered by the incorporation of H 2 DL in the framework of MIL-100(Cr) according to XPS analysis. Our finding provided a novel strategy by constructing defective MIL-100(Cr) and introducing PDVB to enhance efficient adsorption for toluene capture even in humid air.
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Journal of Inorganic and Organometallic Polymers and Materials
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2024
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IF 3.9
Li Mengke,Cao Panpan,Dong Wenwen,Zhao Jun,Li Dongsheng
Organic dyes pollution has caused significant threat to flora, fauna and humans because the toxic of dyes. In this work, with the help of acetic acid as a defect initiator, the hierarchical porous MIL-101(HP-MIL-101) has been synthesized and used for removing anionic dyes Eosin y (EY), Methyl orange (MO), Congo red (CR) and Acid fuchsin (AF) from water. Due to its positive surface charge, larger specific surface area, well-matched pore structure, and the charge, size, and diameter of dyes, HP-MIL-101 showed rapid adsorption and an excellent maximum adsorption capacity of 425 and 336 mg⋅g − 1 for CR and AF, respectively. A series of batch experiments were carried out to investigate the impact of various key factors, including adsorption duration, initial dye concentration, and temperature. In addition, the kinetics, isotherm, and thermodynamics about the adsorption properties were also discussed. In addition, HP-MIL-101 showed stable and high reusability for at least three cycles, with an efficiency of over 95% without significant structural changes. This study highlights the potential of hierarchical porous MOF for mitigating dye pollution and advancing sustainable water treatment methodologies.
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ChemCatChem
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2024
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IF 3.8
Chengzhuo Yu,Jin Xu,Yarui Wang,Silong Wang,Li Xiong,Fanglan Geng,Zesen Shang,Huasheng Wu,Jitao Lv,Lixia Zhao,Yawei Wang
Graphical Untill now, reactive oxygen species (ROS) are difficult to generate in the natural light conditions, since most photocatalysts require external strong stimuli. We surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. The ROS generation patterns and mechanism of MIL-100(Fe)/TiO 2 was revealed by chemiluminescence (CL) and density functional theory (DFT). Reactive oxygen species (ROS), as one kind of the most highly oxidizing oxidants, are difficult to generate and utilize in the natural light conditions, since many materials require external strong stimuli for ROS release to be effective as pollutant degradation or biocide. In this work, we surprisingly found the ROS generation on MIL-100(Fe)/TiO 2 driven by mild natural light. Then ROS generation patterns and mechanism was revealed by chemiluminescence (CL) and density functional theory (DFT). Meanwhile, rhodamine B (RhB) can also be removed by MIL-100(Fe)/TiO 2 under natural light, which further evidence the ROS generation under the natural light. This work provides a new direction for spontaneously generating ROS releasing without external strong stimuli and has the broad potential applications in the field of pollutant degradation or antimicrobials under natural conditions.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2025
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IF 8.5
Le Zhong,Yuxiao Feng,Zichen Wang,Tian Tian,Yali Bi,Jiandong Cui
Enzymatic synthesis of flavor esters is crucial for applications in food, beverage, and cosmetics industries. However, the poor activity and stability of free lipase hinder these reaction. Inspired by the concept of lipase interface activation, MIL-53(Al)-NH 2 was modified with alkyl acid anhydrides of varying chain lengths to tailor its hydrophobicity, and Candida Rugosa lipase (CRL) was subsequently immobilized on this surface to achieve efficient interface activation. The resulting CRL@MIL-53(Al)-AM11 exhibited 3.5 times higher activity than the unmodified CRL@MIL-53(Al)-NH 2 . Moreover, CRL@MIL-53(Al)-AM11 enabled one-step purification of crude CRL via selective adsorption. It also showed enhanced storage and thermal stability as well as higher resistance to protease degradation and denaturants than free CRL. CRL@MIL-53(Al)-AM11 retained 75 % of its initial activity after 30 min treatment at 55 °C, whereas the free CRL retained only 41 %. After 11 days of storage, CRL@MIL-53(Al)-AM11 maintained 70 % of its initial activity, in contrast to 36 % for the free lipase. Notably, CRL@MIL-53(Al)-AM11 achieved a 97 % conversion rate in the esterification synthesis of the flavoring substance (butyl butyrate) within 24 h and retained over 40 % conversion after five consecutive cycles. Therefore, this strategy offers a feasible approach for constructing high-performance immobilized lipases for flavor ester synthesis.
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Journal of Environmental Chemical Engineering
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2024
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IF 7.4
Hao Wang,Renting Huang,Wei Mao,Hao Xu,Chutong Ling,Junru Zhao,Fan Yi,Yongxin Zhou,Jinghong Zhou
Iron-based metal-organic frameworks (MOFs) represent a potentially important tool for controlling organic pollutants . However, the structural stability of most iron-based MOFs in the aqueous environment is limited. Therefore, this study sought to improve the aqueous stability and photocatalytic activity of MIL-101(Fe) using an in-situ modification strategy. A novel and highly water-stable MIL-101(Fe)@IPA 4 was prepared using ligand regulation. Owing to the in-situ modification effect, MIL-101(Fe)@IPA 4 exhibited remarkable hydrophobicity with a water contact angle at 102.4° while maintaining minimal leaching of iron ions (0.46 mg/L), even after five cycles of photocatalysis . Under MIL-101(Fe)@IPA 4 /UV/H 2 O 2 conditions, the removal rates of ciprofloxacin and total organic carbon reached 100% and 49.16%, respectively, within 60 min. These researches suggest that introducing IPA improves the light absorption properties of MIL-101(Fe)@IPA 4 and facilitates electron-hole separation, thereby promoting the generation of active species. The ecotoxicity assessment of major degradation intermediates of ciprofloxacin was conducted using the ECOSAR system. Our findings provide novel insights for enhancing the water stability of iron-based MOFs through an in-situ modification strategy, which is crucial for pollution control efforts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Meidan Que,Peihong Ma,Yabo Wang,Yanbo Sun,Xiangwei Bai,Lili Gao,Jin Chen,Jian Wei,Hui Li
NH 2 -MIL-125 with abundant porosity and specific interactions with CO 2 molecules, has been demonstrate great potential in the field of photocatalytic CO 2 reduction. However, conventional NH 2 -MIL-125 and their composites much lower CO 2 photoreduction efficiency in aerobic environments because of the O 2 competition. To circumvent the issue, this study modifies NH 2 -MIL-125 through crystal facet engineering to enhance its selective CO 2 adsorption and photocatalytic efficiency in the environment of impurity CO 2 . The results indicate that NH 2 -MIL-125 featuring (101) crystal planes can sustain elevated catalytic activity in low-concentration CO 2 environments. In a pure CO 2 atmosphere, NM-5 achieves a CO production rate of 159.66 μmol·g −1 after 4 h, 1.85 times greater than the unmodified NH 2 -MIL-125. Under conditions simulating flue gas (5 % CO 2 ) and ultra-low CO 2 concentrations (0.15 % CO 2 ), NM-5 maintains CO production rates of 3.18 μmol·g −1 and 0.95 μmol·g −1 , respectively, representing 1.63 and 1.73 times the production rates of NM. Furthermore, theoretical calculations indicate that CO 2 exhibits a higher adsorption energy (−1.34 eV) compared to N 2 and O 2 (−0.67 eV and −0.15 eV) on the (101) crystal plane, which reveals the preferential adsorption of CO 2 on the (101) crystal planes. This study involves a novel strategy for optimizing MOFs crystal planes and provides significant insights into achieving efficient photocatalytic CO 2 reduction under aerobic conditions.
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Journal of Inorganic and Organometallic Polymers and Materials
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2025
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IF 4.9
Yu Qinyuan,Li Jiahui,Wang Yufen,Wei Xuedong
Transition metal sulfides (TMS) have drawn increasing research interest owing to their unique electronic structure. They hold broad prospects in accelerating the sluggish oxygen evolution reaction (OER) during water electrolysis. Metal-organic frameworks (MOFs) feature controllable electronic structures and specific surface areas, which facilitate the adsorption of reactants and expedite interfacial electron transfer. Leveraging the above-mentioned advantages of the two materials, a kind of composite electrocatalyst, CuCo 2 S 4 @MIL-53(Fe)/NF, was synthesized by growing MIL-53(Fe) in-situ onto CuCo 2 S 4 nanowires supported on nickel foam. This composite electrocatalyst can accelerate charge transfer, significantly increase the number of active sites, and enhance both electrocatalytic activity and stability. The electrocatalyst CuCo 2 S 4 @MIL-53(Fe)/NF can drive the OER with an overpotential of 390 mV at a current density of 100 mA·cm −2 . Moreover, it still demonstrates excellent catalytic activity after 75 h of testing. This study not only broadens the avenues for sulfide composites but also provides an experimental basis and support for the direct combination of metal chalcogenides and Fe-based MOFs as electrocatalysts.
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