INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Yanping Dong,Xiqiang Tian,Shoulei Huang,Abdullah N. Alodhayb,Muhammad Zahid
The interfacial characteristics of platinum (Pt) metal catalysts can be systematically regulated by interacting them with electropositive metals, leading to synergistic interactions for extensive catalytic applications. In this study, an evenly dispersed polyol-synthesized iron (Fe)-promoted Pt bimetallic nanoparticle (BNPs) system was embedded in MIL-101(Cr). The PtFe 2 @MIL-101(Cr) catalyst unveiled remarkable activity (86%) and selectivity (89%) for the superior hydrogenation of the targeted C O bond of cinnamaldehyde (CAL). The exceptional hydrogenation performance can be credited to the interplay of the geometric and electronic properties arising from charge shuttling between Fe and Pt within the homogenously distributed Pt–Fe bimetallic nanoparticle system. The experimental results indicate enhanced valence electrons in the Pt d-band through the mutual synergetic interface between the Pt and Fe BNPs. Consequently, these Fe–Pt sites functioned as interfacial electrophilic and nucleophilic (Lewis acid-base) sites, enhancing H 2 activation and facilitating C O bond conversion to yield unsaturated cinnamal alcohols (COL). Additionally, the narrow pores of MIL-101(Cr) encapsulating the Pt–Fe BNPs induced steric hindrance, allowing only C O bond hydrogenation. Furthermore, the PtFe 2 @MIL-101(Cr) catalyst maintained its optimal hydrogenation performance over five cycles, demonstrating no substantial loss in either CAL conversion or COL yield, thus endorsing the universal practical applicability of the catalyst.
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高影响因子
JOURNAL OF MATERIALS CHEMISTRY
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2012
·Vol. 22
·期 34
·17833-17841
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IF 5.968
Cheng-Xiong Yang,Xiu-Ping Yan
The adsorption and extraction of fullerenes on the metal–organic framework MIL-101(Cr) were studied in detail in terms of kinetics, thermodynamics, adsorption isotherms, competitive adsorption, and breakthrough curves. The adsorption of C60 and C70 on MIL-101(Cr) follows a pseudo-second-order kinetic model. The adsorption rate constant for C70 is 3 to 5 times that for C60, showing faster and easier adsorption of C70 over C60 on MIL-101(Cr). Intraparticle diffusion model analysis reveals that the adsorption of C60 and C70 on MIL-101(Cr) proceeds by two phases, surface sorption and intraparticle/pore diffusion. The adsorption of fullerenes on MIL-101(Cr) is controlled by entropy changes. The maximum adsorption capacity for C70 at 30 °C (198.4 mg g−1) is 29 times that for C60 (6.76 mg g−1). MIL-101(Cr) shows much more favorable adsorption of C70 and higher fullerenes than C60 with a high selectivity (αC70/C60 = 24). Selective extraction of C70 and higher fullerenes from crude carbon soot can be easily achieved on MIL-101(Cr) via a simple adsorption–desorption process. The used MIL-101(Cr) can be regenerated by washing with o-dichlorobenzene under ultrasonication. The high selectivity, fast adsorption, easy desorption, and excellent reusability makes MIL-101(Cr) attractive as a novel adsorbent for the enrichment and extraction of C70 and higher fullerenes.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
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IF 4.7
Ziyang Xu,Zicheng Yang,Jiale Ni,Yi Feng,Jianfeng Yao
The functionalization of metal organic frameworks (MOFs) with tailored ligands offers a promising pathway for enhancing their catalytic performance in CO 2 fixation. This work systematically explores the impact of ligand engineering in MIL-101(Cr) through carboxyl (–COOH) and amino (–NH 2 ) functionalization for the CO 2 cycloaddition reaction. Comprehensive characterizations of pristine MIL-101 and functionalized MILs involving MIL-101-COOH, MIL-101-NH 2 , and MIL-101-COOH/NH 2 reveal that –COOH functionalization significantly enhances the surface area (2717 m 2 /g) and reduces the activation energy (17.1 kJ/mol vs. 23.1 kJ/mol for pristine MIL-101), whereas –NH 2 groups improve the CO 2 binding strength but compromise the crystallinity and surface area (532 m 2 /g). Under mild conditions (80 °C and 0.1 MPa CO 2 ), MIL-101-COOH achieves >99 % yield for CO 2 cycloaddition with epichlorohydrin at 8 h and maintains stability over ten cycles, outperforming other MILs (72–82.5 % yields). This work establishes ligand engineering, especially –COOH functionalization, as a critical strategy to optimize MILs for CO 2 fixation to produce cyclic carbonates.
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Coatings
·
2025
·Vol. 15
·期 12
·1449
·
IF 2.8
Asen Dimov,George R. Ivanov,Leonard Keil,Andreas Terfort,Jinxuan Liu,Velichka Strijkova
HighlightsWhat are the main findings?A metal–organic Framework (MOF) MIL-101(Cr) with crystal sizes around 20 nm was synthesized and the results were compared to a 300 nm crystal-sized commercially available material.What are the implications of the main findings?Smaller-sized MIL-101(Cr) crystals form a stable insoluble monolayer at the air–water interface with denser, more homogeneous water coverage and packing upon compression, and no visible micrometer-sized aggregates.Langmuir-Blodgett monolayers from the 20 nm MOF show six times lower surface roughness.Metal–Organic Frameworks (MOFs) have diverse applications due to their tunable porosity, large surface area, and diverse chemical functionalities. Among them, one of the most researched MOFs is MIL-101(Cr), which, in addition, is very stable in water. We have used a commercially available substance with approximately 300 nm large crystals for the preparation of a sensing nano-thin layer for the emerging water contaminant PFOS, due to its high selectivity towards this compound. Here, we have synthesized 20 nm sized crystals of MIL-101(Cr), which are among the smallest reported, and compared them to the same material with 300 nm sized crystals. The material was characterized by TEM and XPS. It was possible to prepare insoluble monolayers at the air–water interface (Langmuir films), which were characterized with film compression isotherms, Brewster angle microscopy, and surface potential measurements. The Langmuir–Blodgett (LB) method was used to deposit monolayers on Si wafers and 434 MHz Surface Acoustic Wave resonator simultaneously. The LB layers were very stable over time. The smaller-sized MIL-101 (Cr) crystals exhibit denser, more homogeneous water coverage and packing upon compression, with no observable 10–100 µm aggregates. LB monolayers from the 20 nm particles have approximately six times lower surface roughness. The LB monolayer is far from being smooth, but this will allow excellent access to the MOF pores by the tested analyte in a chemical sensing application. The lack of research on depositing presynthesized MOFs using probably the best method for nanoarchitectonics—the LB method—is addressed. The 20 nm sized MOF crystals are the smallest deposited by this method so far.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Zhaoyang Li,Yongjie Zhao,Qing Guan,Qian Liu,Sara Khan,Leilei Zhang,Xianze Wang,Lei Chen,Xia Yang,Mingxin Huo
Photocatalytic reduction of nitrate has attracted much attention recently, however, low efficiency and difficult separation have limited its application in practice. In this study, the novel direct dual Z-scheme AgBr(Ag)/MIL-101(Cr)/CuFe 2 O 4 (AB/M/CFO) was fabricated by the hydrothermal technology combined with the photodeposition method for the first time. The AB/M/CFO exhibited the highest nitrate conversion and nitrogen selectivity (79.9% and 94.5%, respectively) compared to AgBr(Ag)/MIL-101(Cr), MIL-101(Cr) and CuFe 2 O 4 for 30 min UV-light irradiation. The dual Z-scheme of AB/M/CFO enhanced electron transfer and charge separation, which was proved by transient photocurrent responses, leading to a significant improvement in photocatalytic efficiency. Meanwhile, after four cycles, the AB/M/CFO photocatalyst also displayed a strong magnetic separation ability and excellent recycling stability. Furthermore, the excitation and electron transfer process over dual Z-scheme AB/M/CFO photocatalytic material were proposed, based on the radical trapping experiments. Our work provides a new strategy to construct dual Z-scheme MOFs-based materials that have promising applications in photocatalytic reduction of pollutants.
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SENSORS AND ACTUATORS B-CHEMICAL
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2017
·
IF 5.401
Wanqing Zhang,Zhongyin Zhang,Yuanchao Li,Jun Chen,Xiaobo Li,Yadong Zhang,Yuping Zhang
A novel MIL-101(Cr)/XC-72 modified glassy carbon electrode (GCE) sensor was fabricated to determine chloramphenicol (CAP). The electrochemical sensors were constructed by using MIL-101(Cr), XC-72, MIL-101(Cr)/XC-72, and their electrochemical performances were studied with cyclic voltammetry (CV) and differential pulse voltammetry (DPV) methods. In comparison with the GCE , MIL-101(Cr)/GCE and XC-72/GCE sensors, the MIL-101(Cr)/XC-72/GCE sensor exhibited a well-defined redox peak towards CAP in phosphate buffer solution (PBS). The effects of the ratio of MIL-101(Cr) and XC-72, accumulation time, scan rate, and pH value were carefully considered. Under the optimized conditions, the sensor exhibited excellent response for CAP. The linear concentration ranges of CAP were from 1.0 × 10 −8 to 2.0 × 10 −5 M (R 2 = 0.985), with a low detection limit of 1.5 × 10 −9 M (S/N = 3). Furthermore, the MIL-101(Cr)/XC-72/GCE sensor was successfully applied to the determination of the real samples with satisfactory recoveries.
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TALANTA
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2016
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IF 4.035
Guobin Han,Qiaoling Zeng,Zhongwei Jiang,Tiantian Xing,Chengzhi Huang,Yuanfang Li
Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF-MS) has been proven as a useful and advanced technique in the identification of polymers and proteins. However, MALDI-TOF-MS still has the unavoidable drawback of self-signal interference with traditional organic matrices, which could suppress and overlap with the analyte signals in the low-mass region. In this work, MIL-101(Cr), a kind of metal-organic frameworks which possess high molecular weight , π-conjugated 3-D structure, coordinately unsaturated chromium sites (CUS) and strong absorption in the UV range, was employed to replace traditional organic matrices, and it was found that MIL-101(Cr) can dramatically eliminate the background peaks, showing high signal-to-noise level in the analysis of small molecules. As proof-of-concept, quercetin , daidzein , genistein and naringenin , members of flavonol family which widely exists in food and natural products , were successfully determined by utilizing MIL-101(Cr) as the surface-assisted matrix, and the detection of quercetin was sensitive with good salt tolerance and reproducibility. Under optimal conditions, the mass peak intensity exhibited good linear relationships in the range from 0.25 µg/mL-7.00 µg/mL for quercetin ( R 2 =0.996) with detection limit 2.11 ng/mL (3σ/k), making the identification of quercetin in sophora japonica successfully. With this strategy we have demonstrated the potentiality of MIL-101(Cr) nanomaterials as MALDI-MS matrix for the detection of small molecules.
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PubMed
高影响因子
MICROCHEMICAL JOURNAL
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2025
·
IF 5.1
Jing Meng,Moustafa Zahran,Ahmed S. Abou-Elyazed,Xiaolin Li
Herein, we report a novel electrochemical sensor for determining glucose in sweat, employing a graphene/metal–organic framework (MOF) as a modifier for stainless steel (SS) electrode. The MOF structures, MIL-101(Cr), MIL-101(Cr)-NO 2 , and MIL-101(Cr)-NH 2 , were hydrothermally synthesized and then characterized using X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, N 2 adsorption/desorption isotherms, and scanning electron microscopy (SEM). XRD and SEM results proved the formation of the crystalline MIL-101(Cr) and MIL-101(Cr)-NO 2 , and the amorphous MIL-101(Cr)-NH 2 . Additionally, FT-IR and isotherms confirmed their composition and mesoporosity, respectively. The amorphous MIL-101(Cr)-NH 2 showed the best electrocatalytic activity towards glucose oxidation among the fabricated MOFs. The electrocatalytic activity was also boosted after incorporating conductive graphene. Under optimized conditions, graphene/MIL-101(Cr)-NH 2 /SS was used for glucose determination using square wave voltammetry and chronoamperometry with detection limits of 0.004 and 0.01 mM, respectively. Moreover, the modified electrode showed acceptable recovery values when it was applied to detect glucose in artificial sweat samples.
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JOURNAL OF RARE EARTHS
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2024
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IF 5.2
Xiayu Liang,Aylin M. Deliormanlı,Qingle Zeng
A novel composite material, Poly(IL-AA)@MIL-101(Cr), combining metal-organic framework, polymeric ionic liquid and acrylic acid, was synthesized for the selective and efficient adsorption of rare earths europium(III) (Eu 3+ ). Characterization of the materials was carried out using techniques such as X-ray diffraction (XRD), Fourier transform infrared (FTIR), scanning electron microscopy-energy dispersive X-ray spectroscopy (SEM-EDS), thermogravimetric analysis (TGA) and Brunauer-Emmett-Teller (BET). The results demonstrate successful incorporation of the polymeric ionic liquid onto the material surface while preserving the crystal structure and morphology of MIL-101(Cr). Adsorption experiments were conducted to explore parameters including solution pH, initial Eu 3+ concentration, and duration, with comprehensive analyses of adsorption kinetics, isotherms, and mechanisms. Findings reveal that Poly(IL1-AA)@MIL-101(Cr), Poly(IL3-AA)@MIL-101(Cr), and Poly(IL5-AA)@MIL-101(Cr) achieve adsorption equilibrium for Eu 3+ at approximately 9 h with an equilibrium pH of 6.2. The adsorption of Eu 3+ predominantly follows a pseudo-second-order kinetic model and Langmuir isotherm adsorption model. Moreover, the prepared composite material exhibits superior adsorption selectivity for Eu 3+ over other metal ions in the mixture (K + , Mg 2+ , Ni 2+ , Co 2+ , Zn 2+ , La 3+ , and Nd 3+ ). Even after five adsorption-desorption cycles, the composite material maintains satisfactory adsorption performance.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Guodong Zhang,Zhe Liu,Yaning Kong,Fei Wang
Hydrate-based adsorption and hydration natural gas (AHNG) technology was reported to achieve large methane storage density under mild conditions. In order to enhance methane uptake, a composite nano porous material of MIL-101(Cr)@AC was prepared through fluorine-free hydrothermal reaction, and methane adsorption isotherms for both dry and wet samples were measured under hydrate favorable conditions. Hydrate in-situ formation loaded by the composite material was also carried out, while hydrate kinetics was evaluated by Raman spectrum. It was found that MIL-101(Cr) remains cubic symmetric structure when activated carbon (AC) was doped, but its size decreases with the increase in AC doping amount, while the specific surface area and pore volume significantly increase, and this enhances methane adsorption that increases by 65.58%. More enhanced methane uptake was obtained when wet sample was applied due to adsorption and hydration synergy, wherein methane physical adsorption ability remains, while formed hydrate stores extra methane. The contribution of hydrate to methane uptake is up to 40%, so large methane storage density is anticipated, methane volumetric uptake is up to 179.3 V/V under a mild condition (9.3 MPa and 274.15 K), which increases by 38.03%. Compared with our recently reported ZIF-8@AC, methane storage capacity in this new material increases by 36.5% (Chem. Eng. J., 2023, 455, 140503). In addition, hydrate progressive growth with the increase in adsorption pressure was observed, the area ratio of hydrate large cages to small one finally approaches to the theoretical value of 3:1, suggesting approximately complete conversion of pre-adsorbed water.
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Catalysis Science & Technology
·
2022
·Vol. 13
·期 3
·705-713
·
IF 6.177
Xu Zhang,Xiaoman Li,Senda Su,Mengyao Tan,Guodong Liu,Yingying Wang,Min Luo
The active sites of the catalyst and the charge transfer during the reaction are crucial for the photocatalytic nitrogen reduction reaction (PNRR). Here, ultrafine Ag Nanoparticles (Ag NPs) as the active sites and the electron transporters are successfully fixed in the cavities of the metal–organic frame MIL-101(Cr) by the “double solvent-photoreduction” method. The hydrophilic cages of MIL-101(Cr) could restrict and disperse the growth of Ag NPs, and the windows of the cages prevent them from being detached from the MOF carriers. The Schottky junction between Ag NPs and the MIL-101(Cr) leads to ligand–metal charge transfer (LMCT), while the localized surface plasmon resonance effect (LSPR) possessed by Ag NPs themselves generates hot electrons. Thus, N2 was converted to NH3 by the synergistic effect of the two mechanisms, which was 12 times higher than that of pure MIL-101(Cr) and reached 138.81 μmol g−1 h−1. Furthermore, the mechanism of nitrogen fixation and the reason for the stabilization of this catalyst were investigated, and the results were verified by density functional theory calculations.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Malcom Frimpong Dapaah,Baojian Liu,Liang Cheng
Metal-organic frameworks (MOFs) are of particular interest in the adsorption of organic pollutants . This study investigated the adsorption of aniline (ANI), furfural (FUR), and bisphenol A (BPA) in aqueous solution using MIL-101(Cr)-X (X = –H, –NO 2 , –NH 2 and, –N-2-pyc), MIL-100(Cr, Fe), HKUST-1, and ZIF-8. For the first time, an imino-functionalized MOF was used to adsorb organic compounds in water. MOFs were characterized by XRD, N 2 adsorption-desorption, SEM , TEM, elemental analysis, and FTIR. MIL-101-N-2-pyc demonstrated the highest adsorption capacity of 460.8, 126.5, and 100.7 mg/g towards 500 mg/L BPA, ANI, and FUR respectively. The adsorption isotherms better suited the Langmuir model than the Freundlich model. Importantly, 98% of BPA (100 mg/L) was removed and the kinetic data correlated well with the pseudo-second-order model (R 2 > 0.998). Binary adsorption of FUR and acetic acid (AA) were determined for industrial relevance. MIL-101-N-2-pyc outperformed commercial activated carbon and the other MIL-101s with an impressive co-adsorption of 66.1 mg/g FUR and 62.5 mg/g AA. Overall, the adsorption mechanism was due to hydrogen bonding, π-π interaction, and electrostatic attraction. Moreover, MIL-101-N-2-pyc exhibited remarkable structural stability and less than 0.01 wt% Cr leached into water. The adsorbent regeneration was improved after 4 cycles in methanol.
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