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1.
Inorg Chem ; 59(4): 2171-2177, 2020 Feb 17.
Artigo em Inglês | MEDLINE | ID: mdl-31990539

RESUMO

Glutamate is a biomarker for many nervous system diseases, and sensitively detecting glutamate is meaningful in the clinic. Therefore, a unique 3D framework of Cd-MOF (1) is synthesized and characterized. A single-crystal X-ray study reveals that it is a two-fold interpenetration (4,4)-connected framework with a PtS topology, where a large 1D rhombic channel with a size of 8 × 14 Å exists and the total potential void volume can reach 62%. Luminescence results demonstrate that 1 has good luminescence stability and can sensitively detect glutamate in water with a detection limit of 1.15 × 10-7 mol/L, which makes it the most sensitive MOF-based luminescence sensor of glutamate to date. More importantly, it also can serve as a luminescence sensor to detect glutamate in serum, and the quenching concentration needs to be only 43.1 µmol/L, which is much lower than the harmful level of glutamate (400 µmol/L) in glioma patients' blood. Compound 1 can be used at least five cycles. These results show that 1 has a potential application in monitoring glutamate in clinical scenarios.

2.
Chem Asian J ; 14(20): 3668-3674, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31271258

RESUMO

Two stable heterometal-organic frameworks, {Na[LnCo(DATP)2 (Ac)(H2 O)](NO3 )⋅DMA⋅11 H2 O}n (Ln=Er(1) and Yb(2)), have been prepared with H2 DATP (4'-(3,5-dicarboxyphenyl)-2,2':6',2'''-terpyridine) as organic building block. These two isostructural compounds featuring two-dimensional layer architectures possess outstanding thermal stabilities and excellent chemical stabilities in common organic solvents and different acid/base solutions with pH range changing from 1 to 13. Moreover, compounds 1 and 2 serving as heterogeneous catalysts can efficiently catalyse the CO2 fixation reaction with various aziridines to result in corresponding oxazolidinones at 70 °C. Importantly, a good recyclable performance of 1 for at least 10 cycles is observed based on the experimental results, which are further confirmed by PXRD, TGA and ICP analyses.

3.
Anal Chem ; 91(15): 9754-9759, 2019 Aug 06.
Artigo em Inglês | MEDLINE | ID: mdl-31248252

RESUMO

Colchicine is highly toxic to creatures, and sensitively detecting colchicines is of profound significance in the pharmaceutical, clinical, food, and breeding industries. We herein designed and constructed a unique luminescent indium-organic framework {[(CH3)2NH2][In(L)]·9DMF}n (V105) via an in situ ligand-mediated method, which possesses a 2-fold interpenetrated 3D anionic framework. Due to the large channels that exist in the framework with the size of 12 Å × 14 Å, V105 can rapidly remove harmful cationic dyes from water in a few minutes. Importantly, luminescent experiments demonstrate that V105 can selectively detect colchicine with high sensitivity in water, and the limit of detection can reach 1.0 × 10-7 M. To our knowledge, this is the first example of a metal-organic framework-based luminescent sensor for detecting colchicine.

4.
Anal Chem ; 91(8): 5455-5460, 2019 Apr 16.
Artigo em Inglês | MEDLINE | ID: mdl-30924344

RESUMO

pH value is a key parameter in reflecting the health status, reaction process, and water quality. The construction of highly sensitive pH luminescent ratiometric is important but challenging. Herein we designed and synthesized a unique triple-interpenetrated luminescent lanthanide-organic framework {[Eu(PPTA)0.5(NO3)(DMF)2]·H2O} n(V104) based on an amphoteric ligand 4,4',4'',4'''-(1,4-phenylenebis(pyridine-4,2,6-triyl))tetrabenzoic acid (H4PPTA). Compound V104 possesses high solvent and acid/alkaline stabilities. Luminescent investigations reveal that V104 exhibits dual emission peaks at 390 and 480 nm, and these two peaks can separately detect OH- and H+ among various anions and cations. Importantly, V104 can serve as a self-calibrated pH ratiometric to quantitatively detect pH value, and the sensitivity can reach 403.2% per pH for OH-, and 129.5% per pH for H+. Furthermore, by encapsulating magnetic γ-Fe2O3 nanoparticles in V104, the pH sensor can be readily separated from the analyte by external magnet and recycled at least four times, suggesting as-synthesized γ-Fe2O3@V104 has potential for monitoring pH fluctuations in water. To our knowledge, this is the first self-calibrated ratiometric pH-sensor based on two responsive wave bands which can separately detect OH- and H+.

5.
Angew Chem Int Ed Engl ; 58(2): 577-581, 2019 Jan 08.
Artigo em Inglês | MEDLINE | ID: mdl-30427112

RESUMO

Cyclization of propargylic alcohols with CO2 is an important reaction in industry, and noble-metal catalysts are often employed to ensure the high product yields under environmentally friendly conditions. Herein a porous noble-metal-free framework 1 with large 1D channels of 1.66 nm diameter was synthesized for this reaction. Compound 1 exhibits excellent acid/base stability, and is even stable in corrosive triethylamine for one month. Catalytic studies indicate that 1 is an effective catalyst for the cyclization of propargylic alcohols and CO2 without any solvents under mild conditions, and the turnover number (TON) can reach to a record value of 14 400. Furthermore, this MOF catalyst also has rarely seen catalytic activity when the biological macromolecule ethisterone was used as a substrate. Mechanistic studies reveal that the synergistic catalytic effect between CuI and InIII plays a key role in the conversion of CO2 .

6.
Anal Chem ; 90(3): 1516-1519, 2018 02 06.
Artigo em Inglês | MEDLINE | ID: mdl-29297225

RESUMO

Two novel anionic In-MOFs V101 and V102 were synthesized and structurally characterized. The structrual transformation from 2-fold interpenetration to noninterpenetration was completed by changing solvent from DMF to DEF. Luminescence investigations reveal that only V102 not V101 can sensitively and selectively detect traces of antibiotics nitrofurazone in water solution via an environmentally friendly manner, and the detection limit can reach to 0.2 ppm. The luminescent difference between V101 and V102 mainly originates from the divergence of interpenetration structures. Namely, through interpenetration-control, the luminescent probe can switch on or off to detect nitrofurazone. This is the first example of interpenetration-dependent MOFs-based luminescent probe.

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