DESALINATION
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2022
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IF 11.211
Xiangyunxiu Meng,Ruiwen Luo,Guijie Guo,Yulin Li,Hui Fang,Peng Bai,Jiafei Lyu,Xianghai Guo
Adsorption has been expected to be promising for boron-containing water treatment , boron resources recovery and boron isotopic separation. Although metal-organic frameworks have been demonstrated to be potential adsorbent candidates, in-depth investigation of the structure-performance relationship remains insufficient. Herein, the performance and mechanism of boron adsorption and isotopic separation were systematically investigated with isostructural MOFs. Six isomorphic MIL-100(M) materials with metal species from the third main group (Al, Ga and In) and the fourth period (Sc, Cr and Fe) were solvothermally synthesized as boron adsorbents. Superior boron isotopic separation factors ( S ) with 10 B preference and comparable boron adsorption capacity ( Q ) were observed through batch boron adsorption experiments, where MIL-100(Al) exhibited the highest S of 1.618 and MIL-100(Sc) achieved the largest Q of 8.74 g-B/mol-MOF. A high correlation between metal atomic radius and performance was revealed and a plausible mechanism was proposed for boron adsorption and isotopic separation involving the important role of the metal center through post-adsorption characterization. This study will pave the way for designing boron adsorbents with improved properties and promote the efficient utilization of boron resources in water.
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RENEWABLE ENERGY
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2021
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IF 8.001
Hui Li,Junchi Wang,Xiaoling Ma,Yangyang Wang,Guoning Li,Min Guo,Ping Cui,Wanpeng Lu,Shoujun Zhou,Mingzhi Yu
Solid catalyst loss is inevitable by using the traditional separation methods of centrifugation or filtration. To this end, the carbonized MIL−100(Fe) is used to support ammonium sulfate ((NH 4 ) 2 SO 4 ) for synthesizing magnetic solid acid on the purpose of biodiesel production . Influence of preparation factors of loading amount, activation temperature, and activation time on catalytic activity are initially evaluated. With that, the prepared catalyst (CIS) is comprehensively investigated to obtain the optimal esterification parameters for biodiesel production . Moreover, characterizations of TG, XRD, BET, SEM, EDS, FTIR, py−FTIR, VSM, XPS, and Hammett indicator are conducted to elucidate the structure−function relationship between physicochemical property and catalytic activity . Results indicated the CIS is a superparamagnetism material with the saturated magnetism of 22 emu/g, which could be easily recovered from mixture with external magnet. Furthermore, the maximum conversion of 95.68% is obtained with mild conditions: molar ratio of methanol/oleic acid of 8:1 and catalyst amount of 8 wt% at 70 °C for 2 h. Negligible impact is detected for CIS with presence of 5 wt% water content, even with 20 wt% water content, the conversion of 85.88% is still achieved.
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ACS Applied Nano Materials
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2021
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IF 5.097
Mingqi Xu,Dingzhou Liu,Jinghua Yang,Qian Zhu,Yunliang Wang,Jingquan Sha
Study and application of MIL-100(Fe)-based two-dimensional graphene oxide (GO) nanocomposite was limited because the nucleation of the spherical structure of MIL-100(Fe) on GO along different directions hindered the formation of MOF-100(Fe). To address this issue, MIL-100(Fe)/three-dimensional graphene (3DG) nanocomposites (abbreviated as MIL-3DG-n, n = 25, 50, 75, and 100) were successfully fabricated via in situ growth of MIL-100(Fe) on 3DG matrixes in this work because the unique structure of 3DG can avoid the attachment with MIL-100(Fe) on nucleation sites along multiple directions, resulting in their ideal combination. The prepared MIL-3DG nanocomposites exhibited higher peroxidase-like catalytic activities than pure MIL-100(Fe), and MIL-3DG-75 exhibited the best peroxidase-like activities for detecting xanthine with the detection limit of 0.0014 μM in the linear range of 0–200 μM to date, to the best of our knowledge, which is attributed to the higher affinity of MIL-3DG-75 nanocomposite to peroxidase substrates o-phenylenediamine (OPD) and H2O2, confirmed by the Michaelis–Menten kinetics (Vm: 49.5 × 10–8 M s–1 for H2O2, 18 × 10–8 M s–1 for OPD, Km: 0.029 mM for H2O2, 0.011 mM for OPD). Owing to the high catalytic efficiency of the MIL-3DG-75 nanocomposite, a rapid and efficient strategy for the sensitive colorimetric detection of xanthine was established.
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Surfaces and Interfaces
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2024
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IF 5.7
Pengfei Zhu,Mengrong Geng,Shuang Qin,Heyang Cao,Zhenhong He,Xinhua Gao,Chuanyi Wang
The conversion of CO 2 into chemical products or fuels of great value always remains an outstanding challenge. Here, we report a heterojunction Fe@C/Ni 2 P composite catalyst obtained by preparing MIL-100(Fe) derived Fe@C confined Ni 2 P nanoparticles, which is applied to photothermal catalytic CO 2 hydrogenation with H 2 O. Without adding any sacrificial agents or co-catalysts, the optimal Fe@C/Ni 2 P sample shows higher yields for CO 2 -to-C 2 H 6 and CO 2 -to-CO yield of 5.83 μmol g −1 h −1 and 179.9 μmol g −1 h −1 than that of pristine Fe@C and Ni 2 P, respectively. The experimental results indicated that the obtained Fe@C/Ni 2 P can act as catalytic sites to adsorb, activate, and convert CO 2 under low-intensity LED light irradiation (420 nm) with a temperature of 200 ℃. The physical structure, photochemical properties and energy band structure of the Fe@C/Ni 2 P composite catalysts were investigated by XRD, XPS, FT-IR, TEM, BET, respectively. Furthermore, the reaction pathway of Fe@C/Ni 2 P photothermal catalytic CO 2 hydrogenation with H 2 O to C2 products and CO were systematically analyzed by in situ infrared spectroscopy (DRIFTS).
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JOURNAL OF MATERIALS CHEMISTRY
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2012
·Vol. 22
·期 15
·7449-7455
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IF 5.968
Shu-Hui Huo,Xiu-Ping Yan
The adsorption of malachite green from aqueous solution on a highly porous metal–organic framework MIL-100(Fe) was studied in view of the adsorption isotherm, thermodynamics, kinetics, and regeneration of the sorbent. The adsorption isotherms of malachite green on MIL-100(Fe) followed the Freundlich model, and MIL-100(Fe) possessed heterogeneous surface caused by the presence of different functional groups on the surface. The adsorption of malachite green on MIL-100(Fe) is controlled by an entropy effect rather than an enthalpy change, and obeyed a pseudo-second-order kinetics. Analysis of the intraparticle diffusion plots revealed that more than one process affected the adsorption, and film (boundary layer) diffusion controlled the adsorption rate at the beginning. Evidence from zeta potential and X-ray photoelectron spectroscopic data showed that the adsorption of malachite green was also driven by electrostatic attraction and the interaction between the Lewis base –N(CH3)2 in malachite green and the water molecule coordinated metal sites of MIL-100(Fe). MIL-100(Fe) gave much higher adsorption capacity for malachite green than other conventional adsorbents such as activated carbon and natural zeolite. The high adsorption capacity, good solvent stability, and excellent reusability make MIL-100(Fe) attractive for the removal of MG from aqueous solution.
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JOURNAL OF CHROMATOGRAPHY A
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2017
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IF 3.981
Shu-Hui Huo,Hai-Yan An,Jing Yu,Xue-Feng Mao,Zhe Zhang,Lei Bai,Yan-Feng Huang,Peng-Xin Zhou
In this study, we report a facile, environmental friendly fabrication of a type of magnetic metal-organic framework (MOF) MIL-100 that can be used for magnetic solid-phase extraction (MSPE). The magnetic MOF composites were fabricated using in situ calcination method. The as-synthesized materials exhibited both high porosity and magnetic characteristics. They used for the MSPE of polycyclic aromatic hydrocarbons (PAHs) from water samples. Such MOF-based magnetic solid-phase extraction in combination with gas chromatography equipped with a flame ionization detector (GC-FID), exhibited wide linearity (0.02–250 μ g L −1 ), low detection limits (4.6-8.9 ng L −1 ), and high enrichment factors (452–907) for PAHs. The relative standard deviations (RSDs) for intra- and inter-day extractions of PAHs were ranging from 1.7% to 9.8% and 3.8% to 9.2%, respectively. The recoveries for spiked PAHs (1 μ g L −1 ) in water samples were in the range of 88.5% to 106.6%. The results showed that the special anion-π orbital (electron donor-acceptor) interaction and π-π stacking between magnetic MIL-100 and PAHs play an important role in the adsorption of PAHs.
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PubMed
高影响因子
CATALYSIS COMMUNICATIONS
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2017
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IF 3.33
Bo Xu,Zhiming Chen,Bing Han,Cuncheng Li
This work presents MIL-100(Fe) nanoparticles synthesized using glycol with uniform size and morphology. This is the first report of nanoscale MOFs material synthesized using glycol. The MIL-100(Fe) particles have been characterized by SEM, TEM, XRD and the results indicate that the MOFs particles show monodispersed nanospherical morphology. Photocatalytic study reveals that the MIL-100(Fe) nanospheres exhibit good oxidation ability of benzene to phenol under visible light irradiation with high selectivity.
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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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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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APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Bo Xue,Chuanruo Yang,Pengtao Guo,Ting Wang,Gan Li,Dahuan Liu
The low efficiency of photogenerated carriers separation and slow cycling of Fe 2+ /Fe 3+ in Fe-based metal–organic frameworks (MOFs) have limited the improvement of their photo-Fenton activity. Therefore, in this work, MIL-100/BiOBr heterogeneous photo-Fenton catalyst was constructed by compositing MIL-100 with BiOBr nanosheets through a simple solvent evaporation method. In this system, the type II heterojunctions formed by the close contact of MIL-100 and BiOBr can promote the separation of photogenerated carriers and accelerate the redox cyclic of Fe 2+ /Fe 3+ , thereby significantly enhancing the photo-Fenton activity. Under visible light irradiation for 60 min, the best removal rate of tetracycline hydrochloride (TCH) by MIL-100/BiOBr is 94.3 %. Remarkably, the MIL-100/BiOBr exhibits a nearly fourfold increase in degradation rate constant compared to MIL-100 at photo-Fenton system. In addition, the catalysts can maintain high degradation performance over a wide pH range (3–9) and the co-existence of different anions. An in-depth investigation of the degradation mechanism reveals that superoxide radicals ( · O 2 – ) and hydroxyl radicals (·OH) play major roles in the photo-Fenton system. Based on this, the possible degradation pathways were proposed. Therefore, this study provides a new strategy for Fe-based MOFs to remove emerging pollutants from wastewater by photo-Fenton reaction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2026
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IF 9.1
Yuqi Zhu,Rongbo Li,Zemin Li,Yawei Gu,Rujing Hou,Yichang Pan
Eight silane coupling agents are grafted onto MIL-100(In) membranes for TOL/MCH pervaporation. • Cyclohexyl-configured silane with amine group enables superior TOL/MCH recognition. • Configurational effects maximize binding energy difference, boosting separation factor by 175%. • Two-stage process achieves flux of 402 g·m −2 ·h −1 and separation factor of 8.1. Hydrogen is recognized as a promising green energy carrier, yet its large-scale transportation remains a critical challenge. Toluene/methylcyclohexane (TOL/MCH) serves as a safe and cost-effective liquid organic hydrogen carrier (LOHC), but practical deployment is constrained by inefficient post-dehydrogenation separation. Membrane-based separation offers a potential solution; however, most existing membranes lack sufficient molecular discrimination capability for these two analogues. In this work, MIL-100(In), a metal-organic framework with intrinsic adsorption selectivity toward TOL and MCH, was selected as the membrane substrate. A series of silane coupling agents with and without amino functionality and varying molecular configurations were grafted onto the membrane surface. Remarkably, the three-dimensional saturated cyclohexyl configuration outperforms the planar phenyl group in molecular discrimination among the amino-bearing silanes, overturning the conventional preference for aromatic functionalities. As a result, the separation factor of the MIL-100(In) membrane is enhanced by 175% upon surface modification. Complementary molecular simulations reveal that the spatial configuration of the grafted silane governs the recognition behavior toward aromatic and cycloalkane molecules, as corroborated by binding energy analysis and the minimum intermolecular contact distances obtained from energy-minimized conformations. These findings provide a mechanistic basis for tailoring membrane surface chemistry toward efficient LOHC separation Download: Download high-res image (333KB) Download: Download full-size image
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ANALYTICA CHIMICA ACTA
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2026
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IF 6.1
Peng Zhao,Kai Liu,Yueyan Li,Xiaofang Ban,Yuheng Wu,Jiaqi Liu,Xiaohong Wu,Ziyi Cheng,Fan Wang,Shuo Li,Feng Lin,Huifang Tang,Qingnan Zhao
The excessive activation of sympathetic nerve is closely related to cardiovascular diseases (CVDs). In this study, we developed a novel MIL-100(Fe)@Ag surface-enhanced Raman scattering (SERS) substrate for the simultaneous and effective detection of plasma norepinephrine (NE) and adenosine—two pivotal sympathetic hormones. The microscopic morphology and crystal structure of the substrate were characterized using techniques such as transmission electron microscope (TEM) and X-ray diffraction (XRD). Mechanistically, the HOMO-LUMO energy levels of the detection molecules were calculated using Gaussian. The substrate realized a dual SERS enhancement mechanism through the synergistic effect of localized surface plasmon resonance and interfacial charge transfer. Consequently, the MIL-100(Fe)@Ag platform exhibited high-sensitivity quantitative detection capabilities for NE and adenosine: the detection limit for NE is 0.596 nmol/L; the detection limit for adenosine is 0.24 nmol/L. Crucially, when applied to patients with pheochromocytoma—a neuroendocrine tumor characterized by plasma catecholamine surges, this method achieved robust and stable detection of plasma NE. It offered comparable diagnostic accuracy to conventional mass spectrometry while significantly reducing analysis complexity. Therefore, this innovative strategy may hold great promise for the long-term, decentralized monitoring of sympathetic nerve activity in populations at risk for CVDs or related clinical disorders.
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