CATALYSIS LETTERS
·
2022
·Vol. 153
·期 4
·1159-1169
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IF 2.936
Liang Jilei,Fan Mengwei,Wu Wenjie,Wu Mengmeng,Cai Wangshui,Xinxing Gao,Huang Tingting,Rui Haiyun
This study shows the successful encapsulation of sandwich cobalt–tungsten polyoxomolybdate (Na 12 [WCo 3 (H 2 O) 2 (CoW 9 O 34 ) 2 ], abbreviated as CoWPOM) guest in mesoporous metal–organic framework MIL-101 host under static condition via a facile post-synthesis strategy. Several characterizations including powder XRD, FTIR, TGA, SEM–EDS, UV–vis DRS, XRF, and low temperature N 2 adsorption–desorption isotherm demonstrate the incorporation and homogenous-distribution of the sandwich CoWPOM guests in cavities of the MIL-101 host. The CoWPOM@MIL-101 composite possesses a better synergistic effect, and it demonstrates an excellent oxidative desulfurization catalytic activity with the DBT removal of 98.1% and recyclability at least 5 times without obvious activity decrease. Graphical Abstract
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Tianze Cong,Hui Huang,Hao Zhang,Chengwei Li,Yongpeng Zhao,Zeng Fan,Lujun Pan
In the surface-enhanced Raman scattering (SERS) measurements, it is very important to fabricate “hot spots” and concentrate the analytes into these regions. In this work, a hybrid structure of Au nanostars (NSs) with high SERS sensitivity and metal-organic framework MIL-101(Fe) with high molecular adsorption capability was constructed as high performance SERS substrate. The MIL-101(Fe) shell between AuNSs is several nanometers, promoting the construct of “hot spots” and the aggregation of target molecules. The as-prepared AuNS/MIL-101(Fe) has achieved high SERS sensitivity, long-time stability, reproducibility, and capability of universal detections. The limit of detection for rhodamine 6 G is down to 0.29 nM. Meanwhile, the SERS activity of AuNS/MIL-101(Fe) is kept for at least 30 days. Furthermore, the relative standard deviations of signals on five substrates are all less than 10 %. The as-prepared AuNS/MIL-101(Fe) also exhibit the SERS activities for various molecules including dyes, organic contaminants, pesticides, and amino acids , indicating that the AuNS/MIL-101(Fe) substrates have wide applications in chemical analysis and environmental monitoring.
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JOURNAL OF SOLID STATE CHEMISTRY
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2022
·
IF 3.656
Xiaxi Zhang,Fen Wei,Tao Bao,Sicen Wang
In this study, we report the adsorption removal of indomethacin sodium (IDM) by the mixed-linker Materials of Institute Lavoisier (MIL)-101(Cr)s. The MIL-101(Cr)s were synthesized by controlling the ratios of 1,4-benzene dicarboxylic acid (H 2 BDC) and 2-amino-1,4-benzene dicarboxylic acid (NH 2 –H 2 BDC). Then their adsorption performances toward IDM were investigated. Due to the increase in specific surface area and the contribution of enhanced multiple action mechanisms, MIL-101(20) was proved to have the optimal IDM absorption among all the mixed-ligand MIL-101(Cr)s. The adsorption kinetic data was found to accord with the pseudo-second-order kinetic model, and the rate constant ( k 2 ) was calculated as 0.0059 g mg −1 min −1 . The selected MIL-101(20) exhibited the maximum IDM adsorption capacity of approximately 641 mg g −1 (318 K), calculated from the Langmuir linear plots. The simulation results of the thermodynamic model suggest that the adsorption could be a spontaneous, endothermic process with increasing randomness. The adsorption mechanism analysis indicates that the synergistic effects of electrostatic interaction , hydrogen bond interaction, and π-π stacking could be responsible for efficient IDM adsorption. In addition, the adsorbent also presented good reproducibility over six successive adsorption/desorption cycles. Therefore, the mixed-ligand MIL-101(Cr) could be recommended as a promising adsorbent for the preferential removal of IDM from polluted wastewater.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Sixing Chen,Yi Liu,Yanwei Sun,Guoliang Xu,Taotao Ji,Xiongfu Zhang,Fei Wang,Yi Liu
Concurrent manipulation of orientation and thickness of MOF membranes has become a reliable approach for improving their separation performances. In terms of oriented seeded growth, oriented deposition of MOF nanosheets during seeding process and sealing all intergranular gaps with no discernible increase in membrane thickness during secondary growth have become indispensable. In this study, we pioneered the fabrication of uniform hexagonal-shaped, 20–40 nm thick MIL-96 nanosheets through solvent composition optimization (V H2O /V FA = 1/2). Subsequently, spin coating was employed for c -oriented deposition of uniform MIL-96 seed layer, during which the addition of PVP in the suspension was found to be critical for obtaining qualified seed layer. Finally, well-intergrown, highly c -oriented ultrathin MIL-96 membrane was prepared upon employing NMF as the solvent during secondary growth. Gas permeation results implied that prepared MIL-96 membrane exhibited superior gas separation performance compared with that of a -& b -oriented counterpart.
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Journal of Cleaner Production
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2021
·
IF 9.297
Hong Ma,Yilin Yang,Fengyue Yin,Xiong-Fei Zhang,Jianhao Qiu,Jianfeng Yao
Metal-organic frameworks (MOFs) have been widely explored as adsorbents for heavy metal ions removal. However, the recovery and regeneration of powdery MOFs remains a huge challenge. In this work, MIL-121 (Al-based MOF) crystals were incorporated into biodegradable alginate matrix to form composite beads with enhanced recyclability and adsorption capacity . A systematic adsorption test for Cu 2+ and Cd 2+ was conducted and the optimal sample (with a MOF loading of 50 wt%) presented an adsorption capacity of 204.5 mg/g for Cu 2+ and 88.7 mg/g for Cd 2+ . Moreover, the composite beads can be regenerated effectively by hot water (80 °C). The desorption is attributed to the carboxyl-rich MIL-121, which could release massive protons (H + ) at elevated temperature. Compared with the traditional desorption using strong acids, this chemical-free thermal desorption strategy holds a great potential for adsorbent regeneration and practical wastewater treatment .
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OPTICAL MATERIALS
·
2023
·
IF 3.9
Dedi Liu,Dapeng Dong,Zhenyi Zhang,Yangyang He,Zhenghua Li,Jinhai Niu,Naisen Yu,Hongsheng Jia
Encapsulating organic dyes within porous solids is an efficient way to design luminescent composite materials and devices. However, for practice applications, the luminescence tuning and the stability investigation of such materials is still a challenge work. Here, a comparative in situ Raman spectra and photoluminescence (PL) spectra are employed to study the structural and optical property of both pure Rhodamine B (RHB) and samples absorbed on a kind of typical materials of institute lavoisier frameworks (MIL) under high pressure, respectively. The luminescence of RHB@MIL 53(Fe) can persist to pressures much higher than that for pure RHB. Our studies revealed that the PL emissions of RHB origin from monomeric and dimeric structures, respectively. Furthermore, our results indicated that the confining effect of MIL 53(Fe) pores inhibited the dimerization of RHB molecules under high pressure.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
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IF 5.2
Shirui Pang,Yuxin Liu,Zhe Zhang,Yuxin Li,Chunguang Li,Zhan Shi,Shouhua Feng
The transmembrane diffusion of soluble lithium polysulfides (LiPS) is the main cause of capacity loss and negative electrode corrosion in lithium-sulfur (Li-S) batteries. In order to suppress the shuttle effect of LiPS, a selective permeability membrane was constructed by introducing functional materials with negative charge groups. Herein, a functional separator with high ion conductivity is obtained by casting the environmentally friendly MOF material sulfonic acid functionalized amino-MIL-101 (S-MIL-101) onto the separator. It is found that the functionalized sulfonic acid group not only accelerates the conduction of the lithium-ion but also repels the polysulfide anion through electrostatic interactions . With this functionalized separator, the initial capacity of batteries is 1444.6 mAh·g −1 at 0.2C and remains 990.4 mAh·g −1 after 100 cycles. Meanwhile, the batteries still deliver a high initial discharge capacity of 895.7 mAh·g −1 even with the high-sulfur-loading cathode (4.7 mg cm −2 ) at 0.2C.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2023
·
IF 5.2
Ning Gu,Yueyang Xu,Yan Yin,Xuzhao Gao,Yongping Zeng
SO x released from the combustion of sulfur-containing compounds in fuels pollute the environment and have a serious impact on human health. Adsorption desulfurization is an effective and environmentally friendly technique for removing sulfur-containing compounds from fuels. Metal-organic frameworks (MOFs) have high specific surface areas and can be easily modified and functionalized, making them excellent candidates for adsorption desulfurization in fuels. In this work, the precursor MIL-100(Fe)-SA was prepared using the hydrothermal method , and the adsorbent Ni@MIL-100(Fe)-SA was obtained by doping Ni 2+ into the resulting MIL-100(Fe)-SA using the impregnation method. FT-IR, X-ray diffraction, scanning electron microscopy, transmission electron microscopy and nitrogen adsorption-desorption isotherms were used to analyze the samples. The results indicated that Ni 2+ was successfully loaded onto MIL-100(Fe)-SA, and the MOF's structure remained stable. The adsorption performance of benzothiophene and thiophene was evaluated through batch adsorption experiments. The adsorption capacities of Ni@MIL-100(Fe)-SA for thiophene and benzothiophene were 23.68 mg S/g and 49.58 mg S/g, respectively. These observations could be ascribed to the π-complexation interactions between Ni 2+ of the framework and thiophenic compounds. The regeneration experiments demonstrated that the spent 11Ni@MIL-100(Fe)-SA-1.5 reach 86% of the adsorption capacity of fresh adsorbent after four cycles. Additionally, the regenerated adsorbent maintained good crystallinity after recycling.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 5
·1-8
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IF 5.833
Sun Ying,Lin Tianran,Zeng Cuihong,Jiang Gaoyan,Zhang Xuanhan,Ye Fanggui,Zhao Shulin
A self-correcting fluorescent assay of tyrosinase (TYR) was developed by utilization of Fe-MIL-88B-NH 2 as a peroxidase-like nanozyme and a capture probe. Fe-MIL-88B-NH 2 nanozyme was selected as an electron donor, and the oxidization product (dopamine- o -quinone) acts as an energy acceptor. First, TYR catalyzes the oxidation of tyramine hydrochloride to dopamine and then to dopamine- o -quinone. Second, Fe-MIL-88B-NH 2 with intrinsic peroxidase-like activity decomposes H 2 O 2 to produce ·OH radicals, which further accelerate the oxidation of dopamine to dopamine- o -quinone. Excessive H 2 O 2 and ·OH radicals reduce the interferences from ascorbic acid at the same time providing a self-correcting ability. Dopamine- o -quinone reacts with -NH 2 groups on the ligand of Fe-MIL-88B-NH 2 through Michael reaction which results in fluorescence quenching. Under 365-nm excitation, the fluorescence emission intensity at 452 nm gradually decreased with increasing TYR concentration varying from 0 to 10 U mL −1 . The linear range is from 1 to 5 U mL −1 and the detection limit is 0.05679 U mL −1 . This self-correcting fluorescent assay of tyrosinase exhibits good sensitivity and selectivity which is also successfully applied for tyrosinase inhibitor detection. Graphical abstract
Schematic representation of fluorescent assay for tyrosinase determination based on Fe-MIL-88B-NH 2 nanozyme. A self-correcting fluorescent assay for tyrosinase was developed based on the Fe-MIL-88B-NH 2 nanozyme.
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Wentao Zhang,Wenguang Huang,Jiyuan Jin,Yonghai Gan,Shujuan Zhang
The importance of singlet oxygen ( 1 O 2 ) in synthesis of fine chemicals, inactivation of viruses and bacteria, degradation of pollutants, and photodynamic therapy has promoted the research on photocatalytic generation of 1 O 2 . Metal-organic frameworks (MOFs), owing to the tunable structure, are good candidate photocatalysts for 1 O 2 generation. However, due to the poor visible-light absorption capacity and the invalid recombination of charge carriers, the 1 O 2 generation yields of most MOFs are still limited. Here, we demonstrate that β -diketone anchoring could improve the photocatalytic generation of 1 O 2 by MIL-125 through enhanced energy transfer. The enhanced energy transfer was attributed to both the narrowed bandgap and the diketone-derived oxygen vacancies, which function as the trapping sites for charge carriers. The results here shed light on the generation of 1 O 2 by visible-light-responsive MOFs and provide a new strategy for the design of MOFs-based photocatalysts.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 24
·8540-8548
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IF 4.39
Zixuan Li,Deyi Zhan,Abdul Saeed,Nanjing Zhao,Junfeng Wang,Weihong Xu,Jinhuai Liu
Due to their ultra-thin morphology, larger specific surface area and more exposed active sites, two-dimensional (2D) metal–organic framework (MOF) nanosheets can break the limitations of three-dimensional (3D) MOFs in sensitivity, response speed and the limit of detection for sensing applications. In this work, fluorescent NH2-MIL-53(Al) nanosheets were developed as a fluoride detection sensor compared with the 3D bulk counterpart. The morphological and structural characteristics of the obtained products were systematically characterized, and the favourable chemical and fluorescence stability of the NH2-MIL-53(Al) nanosheets were explored. The fluorescent NH2-MIL-53(Al) nanosheets showed high sensitivity, fast response speed (as short as 10 seconds), low limit of detection (15.2 ppb), and wide linear detection range (5–250 μM), and all performances were better than those of their bulk counterpart. In addition, the sensing mechanism was investigated to be based on the transformation of the NH2-MIL-53(Al) framework that induced the release of fluorescent ligands, resulting in an exceptionally enhanced fluorescence. This work highlights the advantages of 2D MOF nanosheets in fluorescence sensing applications.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Anqi Sun,Ying Wu,Zhenjiang He,Peng Bai,Jiafei Lyu,Xianghai Guo
The flexible metal-organic framework MIL-53(Cr) has been demonstrated to be an efficient adsorbent for liquid phase adsorption and separation, while the effect of this attractive “breathing effect” on its performance remains uncertain. In this research, by increasing the amount of introduced water, MIL-53(Cr) first shrank into a narrow pore form through bound water and then reopened due to the introduction of free water. Using MIL-53(Cr) with diverse amounts of water as an adsorbent, the liquid-phase adsorption and separation of C8 aromatics, including o -xylene (OX), p -xylene (PX), m -xylene (MX) and ethylbenzene (EB), was manipulated by the pre-adsorbed water in MIL-53(Cr). Pre-adsorbing water in MIL-53(Cr) induced a preference reversal between MX and PX, where dry samples preferentially adsorbed MX, while high-water-addition samples preferred PX instead. In addition, the reopened MIL-53(Cr) with high water addition hardly adsorbed EB, thereby increasing the selectivity of xylene isomers to EB. A longer equilibrium time was observed on MIL-53(Cr) with high water addition, during which the adsorption preference shifted from OX to MX to PX. Further molecular simulation provided a microscopic explanation that water molecules in the pores tended to package around MX and EB, hindering their interaction with frameworks or other adsorbates.
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