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1.
J Am Chem Soc ; 146(11): 7159-7164, 2024 Mar 20.
Article in English | MEDLINE | ID: mdl-38467030

ABSTRACT

Here, we report the synthesis of BCN-93, a meltable, functionalized, and permanently porous metal-organic polyhedron (MOP) and its subsequent transformation into amorphous or crystalline, shaped, self-standing, transparent porous films via melting and subsequent cooling. The synthesis entails the outer functionalization of a MOP with meltable polymer chains: in our model case, we functionalized a Rh(II)-based cuboctahedral MOP with poly(ethylene glycol). Finally, we demonstrate that once melted, BCN-93 can serve as a porous matrix into which other materials or molecules can be dispersed to form mixed-matrix composites. To illustrate this, we combined BCN-93 with one of various additives (either two MOF crystals, a porous cage, or a linear polymer) to generate a series of mixed-matrix films, each of which exhibited greater CO2 uptake relative to the parent film.

2.
Chem Commun (Camb) ; 59(50): 7803-7806, 2023 Jun 20.
Article in English | MEDLINE | ID: mdl-37272083

ABSTRACT

Metal-organic frameworks (MOFs) based on high-connected nets are generally very attractive due to their combined robustness and porosity. Here, we describe the synthesis of BCN-348, a new high-connected Zr-MOF built from an 8-connected (8-c) cubic Zr-oxocluster and an 8-c organic linker. BCN-348 contains a minimal edge-transitive 3,4,8-c eps net, and combines mesoporosity with thermal and hydrolytic stability. Encouraging results from preliminary studies on its use as a catalyst for hydrolysis of a nerve-agent simulant suggest its potential as an agent for detoxification of chemical weapons and other pernicious compounds.

3.
Adv Mater ; 35(23): e2209104, 2023 Jun.
Article in English | MEDLINE | ID: mdl-36919615

ABSTRACT

Space cooling and heating, ventilation, and air conditioning (HVAC) accounts for roughly 10% of global electricity use and are responsible for ca. 1.13 gigatonnes of CO2 emissions annually. Adsorbent-based HVAC technologies have long been touted as an energy-efficient alternative to traditional refrigeration systems. However, thus far, no suitable adsorbents have been developed which overcome the drawbacks associated with traditional sorbent materials such as silica gels and zeolites. Metal-organic frameworks (MOFs) offer order-of-magnitude improvements in water adsorption and regeneration energy requirements. However, the deployment of MOFs in HVAC applications has been hampered by issues related to MOF powder processing. Herein, three high-density, shaped, monolithic MOFs (UiO-66, UiO-66-NH2 , and Zr-fumarate) with exceptional volumetric gas/vapor uptake are developed-solving previous issues in MOF-HVAC deployment. The monolithic structures across the mesoporous range are visualized using small-angle X-ray scattering and lattice-gas models, giving accurate predictions of adsorption characteristics of the monolithic materials. It is also demonstrated that a fragile MOF such as Zr-fumarate can be synthesized in monolithic form with a bulk density of 0.76 gcm-3 without losing any adsorption performance, having a coefficient of performance (COP) of 0.71 with a low regeneration temperature (≤ 100 °C).

4.
Pharm Res ; 34(12): 2735-2748, 2017 Dec.
Article in English | MEDLINE | ID: mdl-28913790

ABSTRACT

PURPOSE: HSP90 (Heat shock protein 90kD) has been validated as a therapeutic target in Castrate Resistant Prostate Cancer. Unfortunately, HSP90 inhibitors suffer from dose-limiting toxicities that hinder their clinical applications. Previously developed polymeric delivery systems for HSP90 inhibitors had either low drug content or low biological activity suggesting the need for better delivery system for HSP90 inhibitors. METHODS: We developed a simplified synthetic strategy to prepare polyethylene glycol based water-soluble polymeric system for model HSP90 inhibitor geldanamycin (GDM). We then investigated the effect of cathepsin B degradable linker and drug content in polymeric conjugates on their growth inhibitory property using DU145 (androgen independent) and LNCaP (androgen dependent) cell lines. RESULTS: Water-soluble polymeric conjugates were synthesized with GDM content ranging from 9 to 30% wt/wt. We demonstrated the importance of cathepsin B degradable linker from the context of drug content and different prostate cancer cell lines. The most active conjugate against DU145 cells exhibited IC50 value of 2.9 µM. This was similar to the IC50 (2.1 µM) of small molecular drug aminohexane geldanamycin. CONCLUSION: Water-soluble polymeric conjugate with high drug content was synthesized that exhibited in-vitro growth inhibitory activity similar to small molecular weight HSP90 inhibitor. Graphical Abstract Water soluble degradable polymeric conjugate for the delivery of Geldanamycin.


Subject(s)
Antineoplastic Agents/administration & dosage , Benzoquinones/administration & dosage , Drug Carriers/chemistry , HSP90 Heat-Shock Proteins/antagonists & inhibitors , Lactams, Macrocyclic/administration & dosage , Polymers/chemistry , Antineoplastic Agents/pharmacology , Benzoquinones/pharmacology , Cell Line, Tumor , Humans , Lactams, Macrocyclic/pharmacology , Male , Prostatic Neoplasms, Castration-Resistant/drug therapy , Solubility , Water/chemistry
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