NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 24
·9725-9731
·
IF 3.069
Suresh Mutyala,Sobhy M. Yakout,Shebl S. Ibrahim,Madhavi Jonnalagadda,Harisekhar Mitta
Iron metal–organic framework, MIL-100(Fe) was prepared by a hydrothermal method and used as a support to incorporate diethylenetriamine (DETA) for the study of CO2 adsorption and separation of CO2/N2. All synthesized adsorbents were characterized by PXRD, N2 adsorption–desorption isotherms, FT-IR, TGA, SEM, and elemental analysis. Structural characterization results have revealed that the structure of MIL-100(Fe) was not changed by the incorporation of diethylenetriamine. The CO2 adsorption capacities were 29 cm3 g−1 and 41 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. Adsorption of CO2 on DETA–MIL-100(Fe) was higher than that on MIL-100(Fe). The enhancement was due to the presence of amine groups which could form ammonium carbamate by interaction with CO2. Similarly, the N2 adsorption capacities were 3 cm3 g−1 and 0.9 cm3 g−1 at 298 K, 1 bar for MIL-100(Fe) and DETA–MIL-100(Fe), respectively. The decrease in N2 adsorption capacity was due to the decrease in surface area. The selectivity of CO2/N2 on DETA–MIL-100(Fe) was four times higher than that on MIL-100(Fe). The heat of CO2 adsorption was 74.2 kJ mol−1 at low coverage of CO2 on DETA–MIL-100(Fe) and the CO2 adsorption capacity was constant in each adsorption cycle over the same adsorbent.
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DALTON TRANSACTIONS
·
2015
·Vol. 44
·期 41
·18227-18236
·
IF 4.197
Ruowen Liang,Rui Chen,Fenfen Jing,Na Qin,Ling Wu
H3PMo12O40 molecules have been successfully encapsulated in the cavities of MIL-100(Fe) via a facile hydrothermal method (denoted as HPMo@MIL-100(Fe)). A series of characterization has corroborated the insertion of H3PMo12O40 within the cavities of MIL-100(Fe). The resulting HPMo@MIL-100(Fe) nanocomposites have exhibited much higher photoactivity than the original-MIL-100(Fe) toward the photocatalytic selective oxidation of benzylic alcohols and the reduction of Cr(VI) under visible light irradiation (λ ≥ 420 nm). The higher photoactivity of HPMo@MIL-100(Fe) can be attributed to the integrative effect of enhanced light absorption intensity and more efficient separation of photogenerated electron–hole pairs. The host porous structure of MIL-100(Fe) can achieve a uniform composition with H3PMo12O40, which is significantly important for producing highly reactive dispersed H3PMo12O40 molecules and enhancing the photocatalytic activity of HPMo@MIL-100(Fe) nanocomposites. And the immobilized H3PMo12O40 molecules are more convenient for recycling. Importantly, almost no Fe and Mo ions leach from the MIL-100(Fe) during the reaction, which verifies the photostability of the HPMo@MIL-100(Fe). In addition, possible photocatalytic redox reaction mechanisms have been investigated.
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DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 8
·3467-3477
·
IF 3.3
Wenhui Hu,Zhongxin Song,Lingna Sun,Lei Zhang,Qianling Zhang,Xiangzhong Ren,Yongliang Li
Efficient separation of photogenerated charge carriers is essential for maximizing the photocatalytic efficiency of semiconductor materials in oxygen evolution reactions (OER). This study presents a novel trimetallic photocatalyst, MIL-100(Fe)/TiO2/CoOx, synthesized through a facile microwave-assisted hydrothermal method followed by atomic layer deposition (ALD). The porous MIL-100(Fe) serves as a support for the sequential deposition of TiO2 and CoOx layers via ALD, which enhances electron–hole pair separation and minimizes their recombination. Characterization using transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) confirms the uniform deposition of TiO2 and CoOx layers on the MIL-100(Fe) surface. The optimized photocatalyst, processed with 20 deposition cycles of Co, exhibits exceptional photocatalytic OER performance, with an oxygen evolution rate of 558.3 μmol g−1 h−1. This enhancement in activity is attributed to the synergistic interaction between the spatially separated TiO2 and CoOx cocatalysts, which facilitates efficient charge transfer and increases the number of active sites. These findings highlight the potential of ALD-fabricated heterostructures in the development of advanced photocatalysts for sustainable energy production.
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Water Reuse
·
2024
·Vol. 14
·期 1
·39-50
·
IF 4.3
Huang Yiru,Li Youyou,Zhong Qingwei,Luo Chen
View large Download slide View large Download slide Close modal Metal-organic framework (MOF) materials, characterized by their porosity and large specific surface areas, exhibit excellent adsorption properties. With the aim of removing Te(IV) from environmental aquatic systems, this study is the first to propose the use of MIL-100(Fe). The material reveals a strong adsorption capacity for Te(IV), with maximum adsorption of 531.9 mg/g, superior to other adsorbent materials. Adsorption isotherm and kinetic models indicate that the adsorption process primarily involves monolayer chemical adsorption. According to the thermodynamic parameters, the adsorption reaction is endothermic. The experiment individually examined factors affecting the material's adsorption performance, including adsorbent dose, initial concentration of Te(IV), pH, adsorption time, and coexisting ions. Even under high ion strength conditions and high concentrations of coexisting ions, the material's adsorption efficiency for Te(IV) still reached over 94%. The material has been successfully applied to remove Te(IV) from lake water, river water, and seawater, yielding satisfactory results. Due to the high salinity and ionic strength of the solution, the removal efficiency of Te(IV) in the seawater matrix was slightly lower than that in freshwater (river and lake water). Thus, this material shows promise for the removal of Te(IV) from complex aquatic systems. MIL-100(Fe) was prepared and characterized. The Te(IV) can be adsorbed by MIL-100(Fe) effectively, and the adsorption process was primarily a monolayer chemical adsorption and an endothermic reaction. The Te(IV) can be removed effectively in environmental water supplies by MIL-100(Fe).
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JOURNAL OF MOLECULAR STRUCTURE
·
2025
·
IF 4.7
Zhaobo Wang,Tao Yu,Xiaomao Liu,Jinsheng Li,Xuanwen Liu,Rui Guo
To improve the performance of MIL-100(Fe) in the photo-peroxydisulfate (photo -PDS) degradation system, this study introduced the amino-containing bidentate ligand 5-aminoisophthalic acid (AIA) to simultaneously engineer structural defects and photosensitive sites, thereby synergistically enhancing both photocatalytic activity and metal-mediated catalytic capability. This study synthesized MIL-100(Fe) materials with varying AIA incorporation levels (denoted as M-x %NH₂) and systematically investigated the effects of AIA integration on the catalyst. Degradation experiments were performed in the photo-PDS system using rhodamine B (RhB) as a model pollutant. The results demonstrate that the introduction of AIA induced multiple advantageous effects in the photo-PDS process:1.It enhanced the visible-light absorption capacity;2.Improved the separation efficiency of photogenerated charge carriers;3.Generated defects to increase metal active sites, thereby accelerating PDS activation. Among the samples, M-30 % NH₂ exhibited the optimal performance, achieving nearly complete degradation of RhB within 50 min. The pseudo-first-order rate constant (k) was three times higher than that of unmodified MIL-100(Fe). The catalyst retained approximately 90 % degradation efficiency after five consecutive cycles and demonstrated robust performance across pH 3–9, along with the capability to degrade diverse organic pollutants. Quenching experiments confirmed sulfate radicals (·SO 4 ⁻) and hydroxyl radicals (·OH) as the main active species, and the degradation pathways were elucidated. This study provides foundational insights for modifying MIL-100(Fe) and developing high-efficiency PDS catalysts.
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JOURNAL OF MOLECULAR STRUCTURE
·
2022
·
IF 3.841
Wei Zhang,Yong-Zhuan Zhang,Ji-Min Yang
The separation of synthetic dyes from industrial wastewaters is an important objective in addressing water pollution. The removal of pollutant dyes from industrial wastewater prior to its release into the environment is an essential task; thus, synthesizing new adsorbent materials with superior adsorption efficiency is an important undertaking. Herein, we report the synthesis of MIL-100(Fe)@GO (graphene oxide) composites exhibiting superior adsorption performance toward methyl orange (MO), Congo red (CR), methylene blue (MB), and acid chrome blue K (AC). The room-temperature adsorption capacities of MIL-100(Fe)@GO-1 for these dyes were 533.7 (MB), 760.1 (MO), 1386.3 (AC), and 1786.6 (CR) mg g –1 , exceeding those values previously reported for pristine MIL-100(Fe) by 31.1%, 17.8%, 54.8%, and 8.9%, respectively. The adsorption behavior of the composites can be described on the basis of the structural and morphological characteristics and zeta potential of MIL-100(Fe)@GO and the adsorption capacity and structural characteristics of the dyes. The adsorption uptakes of MIL-100(Fe)@GO toward the pollutant dyes was controlled by the synergistic effects of the hydrogen-bonding, hydrophobic interactions, and π–π interactions and agglomeration pores of MIL-100(Fe)@GO. The obtained results revealed that the synergetic interplay of electrostatic, hydrogen-bonding, π–π, and hydrophobic interactions and adsorption space led to two distinct adsorption regimes for MO and AC depending on the adsorbate concentration.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2020
·
IF 4.551
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
Metal organic frameworks (MOFs) MIL-100(Fe) is considered to be a promising porous adsorbent for dehumidification due to its good hydrophilicity and hydrothermal stability. However, the powdery MIL-100(Fe) prepared by the conventional hydrothermal method is not suitable for industrial rotary desiccant dehumidifier. In order to produce a high-performance rotor core component, a new dry gel conversion in situ synthesis strategy for glass-fiber MIL-100(Fe) monolithic adsorbent was proposed in this paper. The effects of the reaction sol concentration on the crystalline phase, morphology, pore structure , adsorption/desorption performance and the cycling stability of the monolith were discussed in detail. The results showed that MIL-100(Fe) crystals which evenly dispersed in the surface and voids of glass fiber, could be conveniently synthesized in the reaction sols with molar ratios of 1Fe (III)/0.67BTC/xH 2 O (x = 93–185). Among them, the MIL-100(Fe) monolith obtained at x = 93 exhibited a high loading (85.7%), large BET specific surface area (1441 m 2 /g), S-shaped water vapor adsorption isotherm and high saturated adsorption ratio (0.496 g/g) at 298 K and 60% RH , low desorption activation energy (48.28 kJ/mol) as well as a reliable cycling stability. Favorable adsorption/desorption performance of MIL-100(Fe) monolith and convenient dry gel preparation process provide a guidance for the manufacture of high-performance dehumidification rotary wheel.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Yanshu Luo,Bingqiong Tan,Xianghui Liang,Shuangfeng Wang,Xuenong Gao,Zhengguo Zhang,Yutang Fang
With an S-shaped water sorption isotherm and high vapor uptake, as one of the famous metal organic frameworks (MOFs), MIL-100(Fe) (MIL stands for Materials of Institute Lavoisier) has been considered as a very promising candidate for adsorption heat pumps. Usually, MIL-100(Fe) is synthesized by a hydrothermal method under harsh synthesis conditions, such as high temperature and vapor pressure. In this study, in the absence of any solvent, a novel facile MIL-100(Fe) synthetic strategy, which used the dry gel conversion method, was developed. X-ray diffraction (XRD) patterns showed that the new dry gel conversion technology could expediently synthesize MIL-100(Fe) with a low reaction temperature (140 °C) and high yield (85%), which is superior to the hydrothermal method with reaction temperature of 160 °C and yield of 76%. Scanning electron microscopy (SEM) images illuminated that, compared with the conventional synthesized MIL-100(Fe) in the liquid aqueous solution, the new process synthesized one in the dry gel state exhibited a smaller crystal size (about 50 nm) due to the confined growth of the crystals. The pore analysis indicated that the MIL-100(Fe) synthesized by both processes had a similar hierarchical porous structure with the mesopore and micropore; however, compared with the traditional synthesized adsorbent, the new technology synthesized one possessed a larger pore volume due to the formation of the extra mesopores from the interconnection of the nanocrystals. The static adsorption curve exhibited that the water vapor adsorption capacity of MIL-100(Fe) synthesized by the new process was a little higher than the one synthesized by the traditional hydrothermal method. Moreover, it had a smaller desorption activation energy and better cycle stability.
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ChemCatChem
·
2014
·Vol. 7
·期 3
·441-449
·
IF 5.044
Hui Wan,Chong Chen,Zuowang Wu,Yigen Que,Yu Feng,Wei Wang,Lei Wang,Guofeng Guan,Xiaoqin Liu
Graphical Be more active: A new strategy is proposed to construct the ionic liquid, polyoxometalate (POM), and metal–organic framework (MOF) composite. POM bridges the gap between the ionic liquid and the carrier (MOF); thus, the heteropolyanion-based ionic liquid can be encapsulated within the cages of MIL-100 (MIL=Materials of Institut Lavoisier) through anion exchange. The POM–ionic-liquid-functionalized MOF demonstrates high catalytic activity for the esterification of oleic acid with ethanol and is stable in the liquid-phase reaction, with no obvious leaching of the active component. A new strategy was proposed to construct the ionic liquid, polyoxometalate (POM), and metal–organic framework (MOF) composite. The POM-based MOF was synthesized by using the direct hydrothermal method. The sulfonic acid group-functionalized ionic liquid was used for further modification of the hybrid material to realize the encapsulation of the heteropolyanion-based ionic liquid within the cages of the MOF. The catalysts were characterized by using XRD, N 2 adsorption–desorption, FTIR, SEM, TEM, elemental analysis, and TGA. The results indicated that the heteropolyanion-based ionic liquid had been successfully encapsulated within the cages and the structure of MIL-100 (MIL=Materials of Institut Lavoisier) remained intact. The POM–ionic-liquid-functionalized MOF, with high content of the active component, had both Lewis and Brønsted acid sites, which led to high catalytic activity for the esterification of oleic acid with ethanol. The esterification reaction conditions were optimized by using response surface methodology (RSM), and the corresponding conversion of oleic acid reached 94.6 %. The catalyst could be easily recovered and reused six times without significant loss of activity.
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CHROMATOGRAPHIA
·
2024
·
IF 1.2
Shao Xiaozhen,Xu Guangfu,Chen Jiaquan,Miao Pandeng,Yang Ke,Du Yingxiang,Yu Tao
Metal–organic frameworks (MOFs) have a wide range of applications in separation and analytical sciences due to their unique structures. MIL-100(Fe) was immobilized on the inner wall of the capillary column based on the immobilized cysteine (Cys)-triggered in situ growth (ICISG) strategy. By applying this column to capillary electrophoresis, a novel enantioselective separation system based on MIL-100(Fe) nanomaterial was established. By utilizing lactobionic acid (LA) as the chiral selector and optimizing the experimental conditions such as buffer pH, LA concentration and the methanol addition ratio, the CEC system demonstrated a significantly enhanced enantioseparation ability for six basic drugs. The modified capillary column was characterized by scanning electron microscope (SEM), energy-dispersive X-ray spectroscope (EDS) and X-ray diffractometer. The experimental results showed that MIL-100(Fe) was successfully grown on the inner wall of the capillary column. In the present study, the repeatability of the coated column was investigated and the relative standard deviations (RSDs) of the resolution and the migration time for intra-day, inter-day and inter-column were within 8%, proving the good repeatability of the coated column.
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Biomedical Physics & Engineering Express
·
2024
·Vol. 10
·期 4
·045004
·
IF 1.3
Mingjia Feng,Yan Li,Yanfang Sun,Tianqi Liu,Khaydar E Yunusov,Guohua Jiang
The transdermal drug delivery based on microneedles (MNs) provides a suitable and painless self-administration for diabetic patients. In this work, the hydrogel-forming MNs were firstly fabricated using poly(vinyl alcohol) (PVA) and chitosan (CS) as matrix. A hypoglycemic drug, metformin (Met), had been loaded into MIL-100(Fe). Then, both of free Met and Met-loaded MIL-100(Fe) were integrated into hydrogel-forming MNs for regulation of blood glucose levels (BGLs) on diabetic rats. After penetrated into the skin, the free Met could be firstly released from MNs. Due to the absorption of interstitial fluid and subsequent release of loaded Met from MIL-100(Fe), leading to a sustainable and long-term drug release behaviors. A notable hypoglycemic effect and low risk of hypoglycemia could be obtained on diabetic rat models in vivo. The as-fabricated hydrogel-forming MNs expected to become a new type of transdermal drug delivery platform for transdermal delivery of high-dose drugs to form a long-term hypoglycemic effect.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Qi Chen,Xingxing Huang,Cheng Liu,Yueling Chen,Jionghua Wu,Jimmy C. Yu,Ling Wu
The attainment of rapid charge mobility and effective N 2 activation is of critical importance for photocatalytic nitrogen fixation but it has always been a challenge. Such challenge may be met by the construction of a Type II MoS 2 nanoparticles/ MIL-100(Fe) heterojunction photocatalyst. The new material possesses charge migration channels that facilitate the separation of photogenerated carriers. This charge redistribution during photocatalysis is confirmed by experimental results showing a decrease of charge density on the Fe species and an increase of that on Mo. Moreover, DFT calculations show that the adsorption of N 2 and H 2 O is more likely to occur on Fe sites and Mo sites, respectively. These findings clearly suggest a drastically improved spatial isolation of reduction and oxidation sites on the photocatalyst as compared to pristine MIL-100(Fe). The optimized MoS 2 /MIL-100(Fe) exhibits a NH 4 + yield rate of 1.29 μmol·h −1 as excellent utilization of photoinduced electron-hole pairs and effective adsorption and activation of N 2 become possible. This work offers an insight on the synergy of heterojunction engineering with coordinated activation for photocatalytic ammonia synthesis.
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