CRYSTENGCOMM
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2023
·Vol. 25
·期 14
·2110-2118
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IF 3.1
Shi-Jun Yin,Li-Xian Li,Feng-Qing Yang
A polyhedral MIL-125-NH2@Pd nanoparticle with light-responsive oxidase-like activity was synthesized through a simple solvothermal method and was characterized by field emission scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray powder diffraction, Fourier transform infrared spectroscopy, thermogravimetric analysis, Brunauer–Emmett–Teller analysis, etc. MIL-125-NH2@Pd can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) under light radiation without H2O2, indicating its intrinsic light-responsive oxidase-like characteristic. MIL-125-NH2@Pd shows a superior catalytic activity and higher affinity to TMB, compared to MIL-125-NH2, owing to the presence of homogenously distributed palladium (Pd) nanoparticles. The results of the mechanism study indicate the existence of ˙O2− and electron holes during the catalytic reaction of MIL-125-NH2@Pd. Furthermore, based on the excellent light-responsive oxidase-like activity and specific recognition capacity for casein phosphopeptides (CPP) of titanium ions (Ti4+) in MIL-125-NH2@Pd, a simple colorimetric sensing platform was developed for the determination of CPP in a linear range of 10–100 μg mL−1 with a limit of detection as low as 2.9 μg mL−1. Finally, the developed method was successfully employed in the sensitive and selective detection of CPP in spiked rabbit and rat plasma samples. This study may provide a reliable and highly efficient strategy to realize the excitation-responsive sensing applications of materials.
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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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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Yaoxun Zeng,Jiongpeng Yuan,Zhili Ran,Xiaoguang Zhan,Xinyi Li,Huiling Ye,Jiapeng Dong,Guining Cao,Zhenxing Pan,Ying Bao,Junze Tang,Xujie Liu,Yan He
Surgical resection remains the primary treatment modality for bone tumors. However, it is prone to local bone defects and tumor recurrence. Therefore, there is an urgent need for multifunctional biomaterials that combine tumor treatment and bone repair after bone tumor surgery. Herein, a chitosan composite scaffold (CS/DOX@Ti-MOF) was designed for both tumor therapy and bone repair. Among them, the amino-functionalized Ti-based metal-organic framework (NH 2 -MIL-125 (Ti), Ti-MOF) has a high specific surface area of 1116 m 2 /g and excellent biocompatibility, and promotes osteogenic differentiation. The doxorubicin (DOX) loading capacity of Ti-MOF was 322 ± 21 mg/g, and DOX@Ti-MOF has perfect antitumor activity. Furthermore, the incorporation of DOX@Ti-MOF improved the physical and mechanical properties of the composite scaffolds, making the scaffold surface rough and favorable for cells to attach. CS/DOX@Ti-MOF retains the unique properties of each component. It responds to the release of DOX in the tumor microenvironment to remove residual tumor cells, followed by providing a site for cell attachment, proliferation, and differentiation. This promotes bone repair and achieves the sequential treatment of postoperative bone tumors. Overall, CS/DOX@Ti-MOF may be a promising substitute for postoperative bone tumor clearance and bone defect repair. It also provides a possible strategy for postoperative bone tumor treatment.
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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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RSC Advances
·
2021
·Vol. 11
·期 18
·10540-10547
·
IF 3.361
Anxia Li,Xiaoxin Yang,Juan Chen
Metal–organic frameworks (MOFs), such as MIL-53(Fe), have considerable potential as drug carriers in cancer treatment due to their notable characteristics, including controllable particle sizes, high catalytic activity, biocompatibility and large porosity, and are widely used in a broad range of drugs. In this study, a new approach for the synthesis of MIL-53(Fe) nanocrystals with controlled sizes has been developed using a non-ionic surfactant PVP as the conditioning and stabilizing agent, respectively. During the nucleation of MIL-53(Fe), the PVP droplet, as a nano-reactor, controlled the growth of the crystal nucleus. The size and aspect ratio (length/width) of nanocrystals increased with an increase in PVP in the synthetic mixture. The MIL-53(Fe) nanocrystals showed a homogeneous morphology, with approximately 190 nm in length and 100 nm in width. MIL-53(Fe) not only was used to load the anticancer drug doxorubicin (DOX) but also generated hydroxyl radicals (˙OH) via a Fenton-like reaction for ROS-mediated/chemo-therapy of cancer cells. The approach was expected to synthesize numerous types of nano-size iron(III)-based MOFs, such as MIL-53, 89, 88A, 88B and 101. The MIL-53(Fe) nanocrystals hold great promise as a candidate to improve the controlled release of drugs and treatment effect for cancer therapy.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Yixuan Gao,Siming Yan,Yi He,Yi Fan,Liyun Zhang,Jing Ma,Ruitong Hou,Li Chen,Jingyu Chen
Herein, a novel membrane with polyacrylic acid (PAA), NH 2 -MIL-88B(Fe) (NM88B), and graphene oxide (GO) was fabricated via a simple vacuum filter method equipped with the nylon membrane substrate. The composite membrane (PAA@NM88B/GO membrane) retained the laminated structure of GO, and PAA@NM88B was used as the photo-Fenton catalytic nano-filler to intercalate GO. Through a series of material characterization and membrane separation performance tests, the results showed that by introducing porous NM88B and PAA cross-linking modification, PAA@NM88B/GO membrane had excellent hydrophilicity, water flux and dye rejection performance. The flux of the PAA@NM88B/GO membrane was 68.21 L m −2 h −1 bar −1 , which is about 15 times higher than that of GO membrane. In addition, the composite membrane had a high rejection (over 97%) for methylene blue (MB), crystal violet (CV) and Congo red (CR). More importantly, PAA@NM88B/GO membrane can also be used to degrade textile wastewater in real life. The membrane can be used as a catalyst to degrade contaminants, and had a high removal of MB in 40 min (98.79%) under the synergistic effect of membrane adsorption and photocatalysis . Therefore, the results indicated that this new type of PAA@NM88B/GO membrane had potential applications in water purification and actual textile wastewater treatment .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Chaofeng Zhang,Yaozong Yang,Linfeng Li,Jiandong Zhang,Shuangping Huang,Ruifeng Li
Polyoxymethylene dimethyl ether (PODEn) is a promising ether fuel. Especially PODE3–5 can be directly mixed into diesel without modification of the diesel engine’s infrastructure for improving thermal efficiency, and significant reduction in particulate matter (PM) and nitrogen oxides (NOx) emissions. In this paper, a series of heterogeneous catalysts, the imidazole sulfonate ionic liquids (ILs) encapsulated in the cages of metal–organic frameworks (MOFs) MIL-100(Fe), were used successfully and efficiently in the synthesis of polyoxymethylene dimethyl ethers (PODEn) from methanol and trioxane (TOX). These catalysts have exhibited excellent catalytic properties because of strong Brønsted acid sites. MIL-100(Fe)@[BSO3HIm][CF3SO3] shows the best catalytic activity with 96.98% conversation of TOX and 47.49% selectivity of the desired product PODE3–5 under a mild reaction condition. Of importance is that the catalyst is recovered easily and reused.
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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 HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Xiaojuan Li,Fengzhen Liao,Lanmei Ye,Lizhi Yeh
In this study, based on the extensive discussion of the phase transformation process of metal-organic frameworks (MOFs)——MIL-88A(Fe) under thermal treatment, the catalytic performance of MIL-88A-derived iron/carbon (FexC) composites on persulfate (PS) activation for phenol degradation was investigated. FexC-600 ( γ -Fe 2 O 3 /C) exhibited a superior catalytic activity on PS activation for phenol degradation due to higher carbon content, more sp 2 -hybridized structure, carbonyl group and defective sites in composites, in which 98.23% of phenol (20 mg/L) was degraded after 60 min with 0.3 g/L catalyst and 0.3 g/L PS at ambient pH (6.1). The phenol degradation experiments and mechanism studies revealed that there was a catalytic synergism between iron oxides and carbon component in FexC 400-600 composites. Moreover, sulfate radicals (SO 4 − ), hydroxyl radical (•OH), singlet oxygen ( 1 O 2 ) and interfacial electron transfer process all involved in the degradation of phenol by FexC 400-600 composites, but the 1 O 2 -mediated non-radical oxidation was the dominant pathway rather than reactive radicals. Finally, the possible mechanism of PS activation on FexC 400-600 composites was proposed. This work discusses the synergistic catalytic mechanism of FexC composites on PS activation, and favors to provide a better understanding of the metal species and carbon component interaction in iron/carbon-based materials.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 26
·12041-12052
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IF 3.553
Yi Xuerui,He Xiaobo,Yin Fengxiang,Yang Tong,Chen Biaohua,Li Guoru
The global NH 3 production is dominated by Haber–Bosch process, requiring high temperature and pressure. Electrochemical N 2 reduction reaction (NRR) under ambient conditions is a greener path for artificial N 2 fixation to NH 3 but calling for efficient catalyst to increase activity and selectivity. Herein, we report the iron-based metal–organic frameworks (MOFs), i.e., MIL-88B–Fe and amine-functionalized MIL-88B–Fe (NH 2 –MIL-88B–Fe) as efficient catalysts for electrochemical NRR under ambient temperature and pressure in neutral electrolyte. NH 2 –MIL-88B–Fe shows higher NH 3 yield rate of 1.205 × 10 –10 mol s −1 cm −2 than MIL-88B–Fe (3.575 × 10 –11 mol s −1 cm −2 ). Furthermore, NH 2 –MIL-88B–Fe exhibits the highest Faradaic efficiency of 12.45% at 0.05 V versus RHE. The control experiments prove that NH 3 is produced through electrocatalytic NRR. This work may trigger the interest of using MOFs as highly efficient catalysts for electrochemical NH 3 production.
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JOURNAL OF HAZARDOUS MATERIALS
·
2019
·
IF 7.65
Sijia Li,Jianan Cui,Xia Wu,Xuan Zhang,Qi Hu,Xiaohong Hou
Metal-Organic Frameworks (MOFs) are efficient adsorbent and catalyst, however, the prepare of MOFs can be extremely time consuming. The rapid in situ microwave synthesis process offers the possibility of MOFs to a large-scale application. In this study, Fe 3 O 4 @MIL-100(Fe) was rapidly prepared via microwave in 30 min using Fe 3 O 4 as metal precursor and applied as the adsorbent and photocatalyst to remove diclofenac sodium (DCF) from water. Fe 3 O 4 @MIL-100(Fe) exhibited an excellent adsorption effect to DCF with the maximum adsorption capacities of 400 mg/L. The presence of H 2 O 2 could promote the removal of DCF during photocatalytic process. Approximately 99.4% of the DCF was removed in Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 system via adsorption removal and consequent photocatalytic degradation . The high efficiency was attributed to the large BET surface area (1244.62 m 2 /g) and abundant iron metal sites (Fe(III) and Fe(II)) of Fe 3 O 4 @MIL-100(Fe). The adsorptive, photocatalytic property of Fe 3 O 4 @MIL-100(Fe) and the Fenton-like reaction were the main mechanisms for DCF removal. TOC analyzer was served to assess the mineralization of solutions treated by Fe 3 O 4 @MIL-100(Fe)/vis/H 2 O 2 in 12 h. High elimination of TOC (87.8%) was observed during the DCF mineralization process. In addition, the major products were illuminated using HPLC-Q-TOF-MS and DCF degradation pathways were also proposed.
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