A Ti-incorporated metal organic framework structure (MOF) MIL-125, and its amine-functionalized form, NH2-MIL-125, were directly synthesized via a solvothermal route aided by microwave heating, and ...their adsorption (H2O, CO2), separation (isoprene/2-methyl butane) and catalytic properties (olefin cycloaddition, oxidative desulfurization) were investigated. Display omitted
► Titanium-incorporated materials MIL-125 and NH2-MIL-125 were synthesized. ► NH2-MIL-125 was also prepared via microwave heating. ► CO2, N2, and H2O adsorption properties were measured at different temperatures. ► Redox and acid/base catalytic properties were investigated. ► Liquid phase separation of C5 olefin/paraffin was conducted.
A Ti-incorporated metal organic framework structure, MIL-125, and its amine-functionalized form, NH2-MIL-125, were synthesized via a solvothermal route aided by microwave heating. The samples were characterized by XRD, SEM, TGA, EA, UV–vis spectroscopy, and N2 adsorption–desorption measurements. MIL-125 was unstable in aqueous solution, but NH2-MIL-125 was stable both in water and in heptane; its hydrophilic property was further confirmed by water vapor adsorption. NH2-MIL-125 showed moderate CO2 adsorption capacity (136mgg−1) but excellent selectivity over N2 (>27:1) at 298K with a low heat of adsorption surpassing the performance of MIL-125. Four consecutive CO2 adsorption–desorption cycles over NH2-MIL-125 showed completely reversible adsorbent regeneration at 298K under a helium flow for a total duration of 550min. Catalytic properties of the materials were evaluated by cycloaddition of epichlorohydrin and oxidative desulfurization of dibenzothiophene. Finally, batch mode liquid-phase competitive separation of isoprene from 2-methyl butane was conducted, revealing high selectivity of isoprene against 2-methyl butane (ca. 7.8 and 9.7) over MIL-125 and NH2-MIL-125, respectively.
ZIF-8 was synthesized with 85% yield in a 1L vessel using a sonochemical method at high substrate concentration (Zn2+:DMF=1:9.3) in 2h after pH control using triethylamine and NaOH solution. Display ...omitted
► Economic and high yield large scale ZIF-8 synthesis using a sonochemical method. ► Process optimization by systematic investigations on synthesis parameters. ► ZIF-8 pellets using a PVA binder tested for the Knoevenagel condensation reaction.
ZIF-8 was prepared using a sonochemical method under pH-adjusted synthesis conditions using NaOH (aq) with a minimal amount of triethylamine. After optimizing the synthesis parameters, it was extended successfully to 1L-scale synthesis with an 85% product yield at a high substrate concentration (Zn2+:DMF=1:9.3) in 2h without compromising the textural properties. The prepared ZIF-8 samples after pelletization demonstrating excellent catalytic activity in the Knoevenagel condensation reaction of benzaldehyde with malononitrile.
Deoxyribonuclease-I (DNase-I), a representative endonuclease, is an important biomarker for the diagnosis of infectious diseases and cancer progression. However, enzymatic activity decreases rapidly ...ex vivo, which highlights the need for precise on-site detection of DNase-I. Here, a localized surface plasmon resonance (LSPR) biosensor that enables the simple and rapid detection of DNase-I is reported. Moreover, a novel technique named electrochemical deposition and mild thermal annealing (EDMIT) is applied to overcome signal variations. By taking advantage of the low adhesion of gold clusters on indium tin oxide substrates, both the uniformity and sphericity of gold nanoparticles are increased under mild thermal annealing conditions via coalescence and Ostwald ripening. This ultimately results in an approximately 15-fold decrease in LSPR signal variations. The linear range of the fabricated sensor is 20-1000 ng mL
with a limit of detection (LOD) of 127.25 pg mL
, as demonstrated by spectral absorbance analyses. The fabricated LSPR sensor stably measured DNase-I concentrations from samples collected from both an inflammatory bowel disease (IBD) mouse model, as well as human patients with severe COVID-19 symptoms. Therefore, the proposed LSPR sensor fabricated via the EDMIT method can be used for early diagnosis of other infectious diseases.
Many implantable systems have been designed for long-term, pulsatile delivery of insulin, but the lifetime of these devices is limited by the need for battery replacement and consequent replacement ...surgery. Here we propose a batteryless, fully implantable insulin pump that can be actuated by a magnetic field. The pump is prepared by simple-assembly of magnets and constituent units and comprises a drug reservoir and actuator equipped with a plunger and barrel, each assembled with a magnet. The plunger moves to noninvasively infuse insulin only when a magnetic field is applied on the exterior surface of the body. Here we show that the dose is easily controlled by varying the number of magnet applications. Also, pump implantation in diabetic rats results in profiles of insulin concentration and decreased blood glucose levels similar to those observed in rats treated with conventional subcutaneous insulin injections.
Patients with high-risk non-metastatic renal cell carcinoma (RCC) are at risk of metastatic relapse following nephrectomy. Cabozantinib (CZ), a potent multitarget tyrosine kinase inhibitor, ...interferes with angiogenesis and immunosuppression associated with surgery-induced metastasis. Here, we explored the therapeutic potential of CZ-loaded poly(lactic-co-glycolic acid) (PLGA) nanoparticles (CZ-PLGA-NPs) as an adjuvant strategy for targeting post-nephrectomy metastasis. A clinically relevant subline recapitulating post-nephrectomy lung metastasis of high-risk human RCC, namely Renca-SRLu5-Luc, was established through in vivo serial selection of luciferase-expressing murine RCC Renca-Luc cells. CZ was encapsulated into PLGA-NPs via the conventional single emulsion technique. The multifaceted preclinical antimetastatic efficacy of CZ-PLGA-NPs was assessed in Renca-SRLu5-Luc cells. CZ-PLGA-NPs with a smooth surface displayed desirable physicochemical properties, good CZ encapsulation efficiency, as well as controlled and sustained CZ release. CZ-PLGA-NPs exhibited remarkable dose-dependent toxicity against Renca-SRLu5-Luc cells by inducing G2/M cell cycle arrest and apoptosis. CZ-PLGA-NPs attenuated in vitro colony formation, migration, and invasion by abrogating AKT and ERK1/2 activation. An intravenous injection of CZ-PLGA-NPs markedly reduced lung metastatic burden and prolonged lifespan with favorable safety in the Renca-SRLu5-Luc experimental lung metastasis model. The novel CZ-PLGA-NPs system with multifaceted antimetastatic effects and alleviating off-target toxicity potential is a promising adjunctive agent for patients with surgically resected high-risk RCC.
For the prolonged, controlled delivery of systemic drugs, we propose an implantable drug-delivery chip (DDC) embedded with pairs of a microchannel and drug-reservoir serving as a drug diffusion ...barrier and depot, respectively. We pursued a DDC for dual drugs: a main-purpose drug, diclofenac (DF), for systemic exposure, and an antifibrotic drug, tranilast (TR), for local delivery. Thus, the problematic fibrotic tissue formation around the implanted device could be diminished, thereby less hindrance in systemic exposure of DF released from the DDC. First, we separately prepared DDCs for DF or TR delivery, and sought to find a proper microchannel length for a rapid onset and sustained pattern of drug release, as well as the required drug dose. Then, two distinct DDCs for DF and TR delivery, respectively, were assembled to produce a Dual_DDC for the concurrent delivery of DF and TR. When the Dual_DDC was implanted in living rats, the DF concentration in blood plasma did not drop significantly in the later periods after implantation relative to that in the early periods before fibrotic tissue formation. When the Dual_DDC was implanted without TR, there was a significant decrease in the blood plasma DF concentration as the time elapsed after implantation. Biopsied tissues around the Dual_DDC exhibited a significant decrease in the fibrotic capsule thickness and collagen density relative to the Dual_DDC without TR, owing to the effect of the local, sustained release of the TR.
► Content and composition of anthocyanins were evaluated in sweet potato. ► Fifteen individual anthocyanins were isolated and confirmed. ► In steamed tubers, total anthocyanin content was reduced by ...almost half.
As hydrophilic pigments, anthocyanins reduce the incidence of cancer and cardiovascular diseases. In this study, the anthocyanin content and composition following steaming and baking of the roots of the Korean purple-fleshed sweet potato variety “Shinzami” were evaluated using liquid chromatography with diode array detection and electrospray ionisation/mass spectrometry (LC-DAD-ESI/MS). Anthocyanins of Shinzami were composed of mono- or di-acylated forms of p-hydroxybenzoic acid, caffeic acid and ferulic acid with the basic structure of cyanidin 3-sophoroside-5-glucoside or peonidin 3-sophoroside-5-glucoside. A total of 15 individual anthocyanins were isolated and confirmed, one of which was presumed to be a newly identified compound, peonidin 3-feruloyl-p-hydroxybenzoyl sophoroside-5-glucoside. Additionally, the amounts of di-acylated cyanidin 3-caffeoyl-p-hydroxybenzoyl sophoroside-5-glucoside and peonidin 3-caffeoyl-p-hydroxybenzoyl sophoroside-5-glucoside were the highest (137.0 and 565.9mg/100gDW, respectively) among cyanidin and peonidin compounds. After steaming, the total anthocyanin content was reduced by nearly a half, while roasting only slightly reduced the total anthocyanin content.
Prompt administration of first‐aid drugs can save lives during medical emergencies such as anaphylaxis and hypoglycemia. However, this is often performed by needle self‐injection, which is not easy ...for patients under emergency conditions. Therefore, we propose an implantable device capable of on‐demand administration of first‐aid drugs (i.e., the implantable device with a magnetically rotating disk iMRD), such as epinephrine and glucagon, via a noninvasive simple application of the magnet from the outside skin (i.e., the external magnet). The iMRD contained a disk embedded with a magnet, as well as multiple drug reservoirs that were sealed with a membrane, which was designed to rotate at a precise angle only when the external magnet was applied. During this rotation, the membrane on a designated single‐drug reservoir was aligned and torn to expose the drug to the outside. When implanted in living animals, the iMRD, actuated by an external magnet, delivers epinephrine and glucagon, similar to conventional subcutaneous needle injections.
A microneedle (MN) sensor coated with a sensing composite material was proposed for measuring glucose concentrations in interstitial fluid (ISF). The sensing composite material was prepared by ...blending a polymer containing glucose-responsive phenylboronic acid (PBA) moieties (i.e., polystyrene-block-poly(acrylic acid-co-acrylamidophenylboronic acid)) with conductive carbon nanotubes (CNTs). The polymer exhibited reversible swelling behavior in response to glucose concentrations, which influenced the distribution of the embedded CNTs, resulting in sensitive variations in electrical percolation, even when coated onto a confined surface of the MN in the sensor. We varied the ratio of PBA moieties and the loading amount of CNTs in the sensing composite material of the MN sensor and tested them in vitro using an ISF-mimicking gel with physiological glucose concentrations to determine the optimal sensitivity conditions. When tested in animal models with varying blood glucose concentrations, the MN sensor coated with the selected sensing material exhibited a strong correlation between the measured electrical currents and blood glucose concentrations, showing accuracy comparable to that of a glucometer in clinical use.
Chemodynamic therapy (CDT) is based on the production of cytotoxic reactive oxygen species, such as hydroxyl radicals (•OH). Thus, CDT can be advantageous when it is cancer‐specific, in terms of ...efficacy and safety. Therefore, we propose NH2‐MIL‐101(Fe), a Fe‐containing metal–organic framework (MOF), as a carrier of Cu (copper)‐chelating agent, d‐penicillamine (d‐pen; i.e., the NH2‐MIL‐101(Fe)/d‐pen), as well as a catalyst with Fe‐metal clusters for Fenton reaction. NH2‐MIL‐101(Fe)/d‐pen in the form of nanoparticles was efficiently taken into cancer cells and released d‐pen in a sustained manner. The released d‐pen chelated Cu that is highly expressed in cancer environments and this produces extra H2O2, which is then decomposed by Fe in NH2‐MIL‐101(Fe) to generate •OH. Therefore, the cytotoxicity of NH2‐MIL‐101(Fe)/d‐pen was observed in cancer cells, not in normal cells. We also suggest a formulation of NH2‐MIL‐101(Fe)/d‐pen combined with NH2‐MIL‐101(Fe) loaded with the chemotherapeutic drug, irinotecan (CPT‐11; NH2‐MIL‐101(Fe)/CPT‐11). When intratumorally injected into tumor‐bearing mice in vivo, this combined formulation exhibited the most prominent anticancer effects among all tested formulations, owing to the synergistic effect of CDT and chemotherapy.
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