Due to their well-defined 3D architectures, permanent porosity, and diverse chemical functionalities, metal-organic framework nanoparticles (MOF NPs) are an emerging class of modular nanomaterials. Herein, recent developments in the synthesis and postsynthetic surface functionalization of MOF NPs that strengthen the fundamental understanding of how such structures form and grow are highlighted; the internal structure and external surface properties of these novel nanomaterials are highlighted as well. These fundamental advances have resulted in MOF NPs being used as components in chemical sensors, biological probes, and membrane separation materials, as well as building blocks for colloidal crystal engineering.
The development of effective vaccines that can be rapidly manufactured and distributed worldwide is necessary to mitigate the devastating health and economic impacts of pandemics like COVID‐19. The receptor‐binding domain (RBD) of the SARS‐CoV‐2 spike protein, which mediates host cell entry of the virus, is an appealing antigen for subunit vaccines because it is efficient to manufacture, highly stable, and a target for neutralizing antibodies. Unfortunately, RBD is poorly immunogenic. While most subunit vaccines are commonly formulated with adjuvants to enhance their immunogenicity, clinically‐relevant adjuvants Alum, AddaVax, and CpG/Alum are found unable to elicit neutralizing responses following a prime‐boost immunization. Here, it has been shown that sustained delivery of an RBD subunit vaccine comprising CpG/Alum adjuvant in an injectable polymer‐nanoparticle (PNP) hydrogel elicited potent anti‐RBD and anti‐spike antibody titers, providing broader protection against SARS‐CoV‐2 variants of concern compared to bolus administration of the same vaccine and vaccines comprising other clinically‐relevant adjuvant systems. Notably, a SARS‐CoV‐2 spike‐pseudotyped lentivirus neutralization assay revealed that hydrogel‐based vaccines elicited potent neutralizing responses when bolus vaccines did not. Together, these results suggest that slow delivery of RBD subunit vaccines with PNP hydrogels can significantly enhance the immunogenicity of RBD and induce neutralizing humoral immunity.
Adoptive cell therapy (ACT) has proven to be highly effective in treating blood cancers, but traditional approaches to ACT are poorly effective in treating solid tumors observed clinically. Novel delivery methods for therapeutic cells have shown promise for treatment of solid tumors when compared with standard intravenous administration methods, but the few reported approaches leverage biomaterials that are complex to manufacture and have primarily demonstrated applicability following tumor resection or in immune-privileged tissues. Here, we engineer simple-to-implement injectable hydrogels for the controlled co-delivery of CAR-T cells and stimulatory cytokines that improve treatment of solid tumors. The unique architecture of this material simultaneously inhibits passive diffusion of entrapped cytokines and permits active motility of entrapped cells to enable long-term retention, viability, and activation of CAR-T cells. The generation of a transient inflammatory niche following administration affords sustained exposure of CAR-T cells, induces a tumor-reactive CAR-T phenotype, and improves efficacy of treatment.
An in situ method for the preparation of nickel phosphide (Ni 2 P) on silica, alumina, and amorphous silica-alumina (ASA) supports is described. The synthesis avoids the use of nickel and phosphorus salts by employing the reaction between nickel hydroxide (Ni(OH) 2) and hyphosphorus acid (H 3 PO 2), allowing the impregnation of nickel hypophosphite (Ni(H 2 PO 2) 2) onto the oxide supports in the absence of salt byproducts. Temperature-programmed reduction (TPR) in flowing hydrogen at 573-773 K yields phase pure Ni 2 P on the supports with small average particle sizes (3-4 nm) as measured using transmission electron microscopy. The conversion of Ni(H 2 PO 2) 2 to Ni 2 P and related reactions were probed using TPR with on-line mass spectral analysis of the gas effluent. Unsupported Ni(H 2 PO 2) 2 reacts in flowing hydrogen to produce PH 3 and H 2 O at 468 and 482 K, respectively; the reaction is shifted to increasingly higher temperatures for Ni(H 2 PO 2) 2 supported on SiO 2 , Al 2 O 3 and ASA. The hydrodenitrogenation (HDN) and hydrodesulfurization (HDS) properties of the Ni 2 P catalysts were probed using a mixed feed containing carbazole and benzothiophene. While Ni 2 P/SiO 2 catalysts prepared by the different methods exhibited similar HDN and HDS activities, the in situ prepared Ni 2 P/Al 2 O 3 and Ni 2 P/ASA catalysts were substantially more active than their ex situ counterparts prepared from hypophosphite-and phosphate-based precursors.
An allosterically regulated, asymmetric receptor featuring a binding cavity large enough to accommodate three-dimensional pharmaceutical guest molecules as opposed to planar, rigid aromatics, was synthesized via the Weak-Link Approach. This architecture is capable of switching between an expanded, flexible "open" configuration and a collapsed, rigid "closed" one. The structure of the molecular receptor can be completely modulated in situ through the use of simple ionic effectors, which reversibly control the coordination state of the Pt(II) metal hinges to open and close the molecular receptor. The substantial change in binding cavity size and electrostatic charge between the two configurations is used to explore the capture and release of two guest molecules, dextromethorphan and β-estradiol, which are widely found as pollutants in groundwater.
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