CHEMOSPHERE
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2022
·
IF 8.943
Lu Zheng,Yifan Gu,Baolv Hua,Jiarui Fu,Fengting Li
Metal-organic frameworks have been investigated in Fenton-like catalysis for tetracycline hydrochloride degradation, a widely used antibiotic which threatens the growth and health of creatures. However, powder phase and absence of large pores limit the materials’ degradation performance and application. In this work, a hierarchical macro-meso-microporous composite melamine sponge@MIL-101-Fe-NH 2 was firstly designed and constructed. While the micropores provided plenty of active sites to generate reactive oxygen species , the macropores and mesopores accelerated mass transfer. Besides, MIL-101-Fe-NH 2 particles dispersed on melamine sponge individually, exposing more catalytic sites and avoiding inactivation caused by aggregation compared to powder catalysts. Its catalysis performance for tetracycline hydrochloride degradation was evaluated through changing various influence factors like H 2 O 2 concentration, catalyst amount, pH and coexisting ions. Different from the preference of homogenous Fenton catalysts for pH 2–4, the composite displayed the most effective degradation at a subacid environment closer to nature with 77.24% in 30 min. Owing to the synergistic effect of hierarchical porous structure and monodispersed nanoparticles , the composite exhibited faster reaction rate and longer persistence compared to powder MIL-101-Fe-NH 2 . Easy recycling and less ion leaching made it advantages for practical application. •OH, •O 2 − and 1 O 2 active species contributed together to the degradation and two main possible degradation pathways were put forward based on 35 detected intermediates.
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高影响因子
JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2022
·Vol. 331
·期 2
·889-902
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IF 1.754
Fu Xibiao,Liu Jun,Ren Zheng,Zhang Siqin,Xiao Fangzhu,Peng Guowen
Metal-organic frameworks (MOFs) MIL-101(Cr)-PMIDA with phosphate groups were prepared for the adsorption of U(VI). The morphology and structure of the samples were characterized by SEM, TEM, FT-IR, BET, XPS and XRD. This study investigated the effects of the initial U(VI) concentration, contact time, pH, adsorption temperature and coexisting ions on the adsorption of U(VI) by MIL-101(Cr)-PMIDA. The experimental results showed that the adsorption capacity of MIL-101(Cr)-PMIDA was 267.92 mg g −1 at C 0 (U) = 40 mg L −1 , pH = 6.0 and T = 298 K, which was much higher than that of MIL-101(Cr)-NH 2 (71.10 mg g −1 ). More importantly, the material exhibited excellent selective removal performance for U(VI) in an aqueous solution. Furthermore, adsorption thermodynamics and kinetic studies showed that the adsorption was spontaneous (∆G < 0) and exothermic (∆H ˃ 0), following the pseudo-second-order kinetic model (R 2 > 0.99). Graphical abstract
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 46
·期 5
·2309-2319
·
IF 3.591
Yichen Jiang,Yifei Zhao,Lin Liang,Xiao Zhang,Jianmin Sun
Imidazolium-based ionic liquid 1,n-dialkyl-3,3′-bis-1-vinyl imidazolium dibromide (n = 2, 4 and 6) monomers were synthesized and further polymerized inside a MIL-101 framework to afford poly(ionic liquid)@MIL-101 composites (PIL-n@MIL-101, n = 2, 4 and 6). Furthermore, the ratio of poly(ionic liquid) to MIL-101 affected the structures of the composites. Different molar ratios of PIL-4/MIL-101 were prepared and characterized using elemental analysis, powder X-ray diffractometry, thermogravimetric measurements, N2 adsorption/desorption and CO2 adsorption measurements. Thanks to the high Brunauer–Emmett–Teller surface area and porous structure of MIL-101 together with the incorporated poly(ionic liquid), PIL-4@MIL-101-0.5 exhibited good CO2 uptake capacity (42.7 cm3 g−1 at 100 kPa, 273 K). Additionally, due to the synergistic effects of the unsaturated coordinated Lewis acidic Cr sites and nucleophilic Br− in the PIL-4@MIL-101 composites, the developed composites exhibited efficient catalytic performance in the CO2 and epichlorohydrin cycloaddition reaction, with 99.6% conversion obtained at 90 °C and 1.0 MPa for 2.5 h without an additional cocatalyst or solvent. The composites also showed easy separation and better recycling stability. Combining the advantages of facile synthesis, excellent performance for CO2 adsorption and conversion, good thermal stability and recycling stabilities, the poly(ionic liquid)@MIL-101 composites are appealing candidates for application in CO2 capture and utilization.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xueying Wang,Qian Ma,Yi Wang,Dongheng Zhao,Lingyu Li,Huayushuo Zhang,Bolong Li
This study originally reports the in-situ construction of porous WO 3 /FeWO 4 ribbon-like hierarchical composites with unique and intense heterojunction interface behavior and the enhanced adsorption and carrier transport capability for effectively detecting n-butanol at room temperature. The introduction of different adding amounts of MIL-101 plays the key role of the morphological evolution of WO 3 -based microstructures with the well-distributed nanoparticles in situ growth on the surface by a facile electrospinning and subsequent calcination process. Compared with pristine WO 3 , a sharp and useful reduction of the optimal operating temperature from 220 to 25 °C can be observed as the Fe component increasing, mainly owing to the inverted p-type gas sensitive response caused by the controllable variable of FeWO 4 phase in the multiple effective WO 3 -FeWO 4 heterojunctions . The optimal WO 3 /FeWO 4 composites can display the highest response of 12.3 and a relatively short response/recovery times of 110/140 s to 100 ppm n-butanol at 25 °C, together with the superior gas selectivity, repeatability, humidity and long-term stability. Density functional theory (DFT) simulation is employed for verifying the significant adsorption interaction and charge transfer between n-butanol molecule and WO 3 /FeWO 4 . Regular distribution of WO 3 -FeWO 4 heterojunction interfaces can not only determine the collaborative modulation of electronic structures, but also provide the efficient surface/interface transport mechanism for MIL-101 induced one-dimensional (1D) hierarchical ribbons. Actually, the integrated gas-sensitive components based on WO 3 /FeWO 4 composites exhibit the rapid response characteristic under room temperature condition and provide a friendly strategy of optimizing the practical detection of ppm-level n-butanol for other inorganic heterogeneous sensors.
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INORGANICA CHIMICA ACTA
·
2021
·
IF 2.545
Ji-Min Yang,Yun-Kai Kou
Metal-organic framework-based composites can help overcome the functional shortcomings of single materials by virtue of the synergetic properties of their components. The new functionalities introduced in the resulting material allow for their use in a wide range of applications. Herein, we prepared a fluorescent amino-CQDs@MIL-101-SO 3 H composite sensor by immobilizing amino-functionalized carbon quantum dots (amino-CQDs) on sulfo-modified MIL-101 nanoparticles. MIL-101-SO 3 H was not only used as a carrier to encapsulate the amino-CQDs in the pore cavity by hydrogen bonding interactions between the free -SO 3 H groups of MIL-101-SO 3 H and the –NH 2 group of the amino-CQDs, but also as an adsorbent to selectively adsorb and capture the target analyte, i.e. 2,4-dinitrophenol (DNP), via hydrogen bonding interactions between the free -SO 3 H groups of MIL-101-SO 3 H and the –NO 2 group of DNP. The amino-CQDs were used as a probe to sense the target molecules with high selectivity. The amino-CQDs@MIL-101-SO 3 H composite sensor displayed excellent selectivity and sensitivity toward DNP, with a detection limit of 0.041 μM. This is the first study to demonstrate the immobilization of fluorescent amino-CQDs in mesostructured MIL-101-SO 3 H. The selective fluorescence detection demonstrated herein will provide a new platform for sensing hazardous pollutants.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2021
·Vol. 22
·期 19
·10412
·
IF 5.924
Huiping Chen,Yongpan Shan,Lidong Cao,Pengyue Zhao,Chong Cao,Fengmin Li,Qiliang Huang
Long-term use of a single fungicide increases the resistance risk and causes adverse effects on natural ecosystems. Controlled release formulations of dual fungicides with different modes of action can afford a new dimension for addressing the current issues. Based on adjustable aperture and superhigh surface area, metal–organic frameworks (MOFs) are ideal candidates as pesticide release carriers. This study used Al3+as the metal node and 2-aminoterephthalic acid as the organic chain to prepare aluminum-based metal–organic framework material (NH2-Al-MIL-101) with “cauliflower-like” structure and high surface area of 2359.0 m2/g. Fungicides of azoxystrobin (AZOX) and diniconazole (Dini) were simultaneously encapsulated into NH2-Al-MIL-101 with the loading content of 6.71% and 29.72%, respectively. Dual fungicide delivery system of AZOX@Dini@NH2-Al-MIL-101 demonstrated sustained and pH responsive release profiles. When the maximum cumulative release rate of AZOX and Dini both reached about 90%, the release time was 46 and 136 h, respectively. Furthermore, EC50values as well as the percentage of inhibition revealed that AZOX@Dini@NH2-Al-MIL-101 had enhanced germicidal efficacy against rice sheath blight (Rhizoctonia solani), evidenced by the synergistic ratio of 1.83. The present study demonstrates a potential application prospect in sustainable plant protection through co-delivery fungicides with MOFs as a platform.Keywords:NH2-Al-MIL-101;controlled release;dual encapsulation;synergistic effect;rice sheath blight
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Mengtian Jia,Yanyan Zhu,Dong Guo,Xiaogang Bi,Xiaohong Hou
Core-shell magnetic Fe 3 O 4 @MIL-101(Cr) nanoparticles were synthesized via layer-by-layer self-assembly method. Using Fe 3 O 4 @MIL-101(Cr) as support, Fe 3 O 4 @MIL-101(Cr)@MIP was prepared with phenytoin as template, acrylamide as functional monomer , ethylene glycol dimethacrylate as cross-linker, methanol and acetonitrile as porogen , azoisobutyronitrile as initiator. The materials were characterized by a serious of characterization experiments. The prepared Fe 3 O 4 @MIL-101(Cr)@MIP was demonstrated to possess good separability, large adsorption capability, excellent adsorption selectivity , good durability and reusability via adsorption experiments. Subsequently, a magnetic solid phase extraction method (MSPE) based on Fe 3 O 4 @MIL-101(Cr)@MIP combined with high performance liquid chromatography-ultraviolet detector (HPLC-UV) was established for the determination of phenytoin sodium in plasma samples. Experimental parameters including pH, the amount of adsorbent, extraction time, elution conditions, the concentration of NaCl were investigated to optimize extraction process. The method was validated. The linearity was observed in the range of 0.05–40 μg mL −1 with a lower limit of quantification of 0.05 μg mL −1 . The calibration equations were y = 0.2514x + 0.0319 ( r 2 = 0.9938), y = 0.2888x + 0.0472 ( r 2 = 0.9943), y = 0.2565x + 0.0418 ( r 2 = 0.9976), respectively. The recoveries ranged from 89.2 to 94.3%, intra- and inter-day precision (RSDs) ranged from 2.1 to 9.7% and 2.9–9.2%, respectively. The established MSPE-HPLC-UV method was time-saving, sensitive, accurate, environmental friendly, and drastically reduced the complex matrix interferences. The established method was successfully applied for phenytoin sodium determination in real plasma samples, providing new directions for therapeutic drug monitoring.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Sen Xu,Meng Wang,Bo Feng,Xinchen Han,Zijie Lan,Huajun Gu,Hexing Li,Hui Li
Dynamic kinetic resolution (DKR) of amines is an important strategy for the synthesis of chiral drugs and their building blocks; however, improving the matchability of metal-catalyzed racemization and enzymatic resolution is still a task. In this paper, Pd nanoparticles (NPs) were encapsulated inside the cages of ethylenediamine-grafted MIL-101 (ED-MIL-101), giving highly efficient catalysts (Pd/ED-MIL-101) for the racemization of primary amines. The racemization can be combined with lipase-catalyzed resolution in a one-pot DKR of rac -1-phenylethylamine leading to optically pure product (>99% ee value) with an excellent conversion and selectivity up to 99% and 93%, respectively, superior to other catalysts, such as Pd/MIL-101, Pd/MCM-41 and commercially available Pd/C. Furthermore, the heterogeneous chemoenzymatic catalyst combination can be recovered and recycled 8 times without significant loss of efficiency. The enhance catalytic performances were found to depend on the amine modification of MIL-101 that not only endows the surface of its cages with basic property, but also enables efficiently confining Pd NPs in the cages. In addition, the matchability of such chemoenzymatic catalyst combination can be further enhanced by conducting the DKR process under microwave irradiation.
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Nano Life
·
2015
·
IF 0
Qiong Yi,Ling Li,Wei Hong,Lu Fan
A composite of chromium (III) terephthalate metal-organic framework and graphene oxide (MIL-101/GO) coated stir bar was prepared by sol–gel technique for the first time and was employed for stir bar sorptive extraction (SBSE) of trace azo dyes amaranth, sunset yellow and carmine from water samples followed by UV–Vis spectrophotometric detection. A MIL-101/GO coating was first created on the glass bar surface. MIL-101/GO and MIL-101/GO coated stir bars were characterized. The enrichment factors of azo dyes by SBSE have been investigated in detail, and the optimized experimental parameters were obtained. Under the optimal conditions, a method for determination of trace amount of azo dyes was setup, and the detection limits of amaranth, sunset yellow and carmine were 2.3 ng/mL, 1.7 ng/mL and 1.6 ng/mL. The proposed method was successfully applied for the analysis of the three azo dyes in water samples.
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CHEMICAL PAPERS
·
2017
·Vol. 72
·期 1
·235-250
·
IF 1.258
Duan Mei-Juan,Guan Ze-yu,Ma Yong-Wen,Wan Jin-Quan,Wang Yan,Qu Yan-Fei
In this work, effective and novel heterogeneous catalysts of Metal–organic framework MIL-101(Fe) doped with cobalt (Co 2+ ) or copper (Cu 2+ ) have been synthesized by post-synthesis method, namely Co–MIL-101(Fe) and Cu–MIL-101(Fe). The initial and metal-doped samples were tested to activate persulfate (PS) for removal of Acid Orange 7 (AO7) in water. The surface of samples were characterized using X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, N 2 adsorption, scanning electron microscopy and transmission electron microscopy. The addition of Cu 2+ and Co 2+ could alter structure characteristics of MIL-101(Fe) in crystal structure and morphology. The unusual octahedron morphology of MIL-101(Fe) turned to be irregular, disorder and a rod-like morphology was shaped. What is more, Co doping caused greater changes in structure characteristics in comparison with Cu doping. The alteration was reflected in the catalytic capacity of PS activation. An interesting note was that, whether Co or Cu doping, metal-doped MIL-101(Fe) greatly improved the PS activation as compared to unmodified MIL-101(Fe). The removal rate of AO7 was about 66, 92, 98% in MIL-101(Fe)/PS, 6%wtCu–MIL-101(Fe)/PS and 6%wtCo–MIL-101(Fe)/PS system, respectively. Some results also suggested the performance of Co–MIL-101(Fe) was superior to that of Cu–MIL-101(Fe). Additionally, a series of parameters were designed to achieve maximum capacity of PS activation. Such an enhancement in activity may be attributed to the main reasons: the new active sites created by metal additives; an increase in number of active Fe sites produced by Co and Cu doping which results in alteration of morphology and structure of catalysts.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2016
·Vol. 23
·期 15
·15218-15226
·
IF 2.76
Yue Xinxin,Guo Weilin,Li Xianghui,Zhou Haihong,Wang Ruiqin
In this study, a novel core-shell Fe 3 O 4 @MIL-101 (MIL stands for Materials of Institute Lavoisier) composite was successfully synthesized by hydrothermal method and was fully characterized by X-ray diffraction, transmission electron microscopy, Fourier-transform infrared spectra, and X-ray photoelectron spectroscopy. The composite was introduced as a catalyst to generate powerful radicals from persulfate for the removal of Acid Orange 7 in an aqueous solution. Effects of the central metal ions of MIL-101, amino group content of MIL-101, and pH were evaluated in batch experiments. It was found that both hydroxyl and sulfate radicals were generated; importantly, sulfate radicals were speculated to serve as the dominant active species in the catalytic oxidation of Acid Orange 7. In addition, a possible mechanism was proposed. This study provides new physical insights for the rational design of advanced metal-organic frameworks (MOF)-based catalysts for improved environmental remediation.
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RSC Advances
·
2017
·Vol. 7
·期 39
·24453-24461
·
IF 3.108
Chaocheng Zhao,Pei Dong,Zongmei Liu,Guangrui Wu,Shuaijun Wang,Yongqiang Wang,Fang Liu
An active Fe3O4/MIL-101 hybrid material was prepared via a simple in situ solvothermal method and characterized as a heterogeneous Fenton-like catalyst for Rhodamine B (RhB) degradation. The Fe3O4/MIL-101 exhibited enhanced catalytic performance for RhB degradation in a neutral solution. Under optimized conditions, almost 100% removal of 10 mg L−1 RhB was achieved in 30 min using 0.5 g L−1 Fe3O4/MIL-101 and 20 mM H2O2 at initial pH 7. The reusability of Fe3O4/MIL-101 was also investigated after four runs. On the basis of the characterization of the catalyst, the results of metal leaching, the effects of radical scavengers, and hydroxyl radical (˙OH) determination, it was concluded that RhB is decomposed mainly by the attack of the hydroxyl radical (˙OH), generated by the reaction of Fe2+ species with H2O2. MIL-101 showed a significant synergistic effect with Fe3O4, in which it played the role of a solid-acid catalyst with Lewis acid sites on its surface, ensuring that a Fenton-like reaction occurred in the neutral solution.
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