Owing to their large ratio of surface area to mass and volume, metal-organic frameworks and porous carbons have revolutionized many applications that rely on chemical and physical interactions at ...surfaces. However, a major challenge today is to shape these porous materials to translate their enhanced performance from the laboratory into macroscopic real-world applications. In this review, we give a comprehensive overview of how the precise morphology control of metal oxides can be transferred to metal-organic frameworks and porous carbon materials. As such, tailored material structures can be designed in 0D, 1D, 2D, and 3D with considerable implications for applications such as in energy storage, catalysis and nanomedicine. Therefore, we predict that major research advances in morphology control of metal-organic frameworks and porous carbons will facilitate the use of these materials in addressing major needs of the society, especially the grand challenges of energy, health, and environment.
We give a comprehensive overview of how the morphology control is an effective and versatile way to control the physicochemical properties of metal oxides that can be transferred to metal-organic frameworks and porous carbon materials.
The development of metal‐organic frameworks (MOFs) has had a significant impact on various fields of chemistry and materials science. Naturally, polymer science also exploited this novel type of ...material for various purposes, which is due to the defined porosity, high surface area, and catalytic activity of MOFs. The present review covers various topics of MOF/polymer research beginning with MOF‐based polymerization catalysis. Furthermore, polymerization inside MOF pores as well as polymerization of MOF ligands is described, which have a significant effect on polymer structures. Finally, MOF/polymer hybrid and composite materials are highlighted, encompassing a range of material classes, like bulk materials, membranes, and dispersed materials. In the course of the review, various applications of MOF/polymer combinations are discussed (e.g., adsorption, gas separation, drug delivery, catalysis, organic electronics, and stimuli‐responsive materials). Finally, past research is concluded and an outlook toward future development is provided.
The combination of metal‐organic frameworks (MOFs) and polymers in various fields of research is highlighted. MOF‐governed polymerization catalysis and MOFs as a polymerization environment are covered, and the work on MOF/polymer composites and hybrid materials with respect to bulk materials, membranes, and dispersed materials are presented.
The stress response is an essential mechanism for maintaining homeostasis, and its disruption is implicated in several psychiatric disorders. On the cellular level, stress activates, among other ...mechanisms, autophagy that regulates homeostasis through protein degradation and recycling. Secretory autophagy is a recently described pathway in which autophagosomes fuse with the plasma membrane rather than with lysosomes. Here, we demonstrate that glucocorticoid-mediated stress enhances secretory autophagy via the stress-responsive co-chaperone FK506-binding protein 51. We identify the matrix metalloproteinase 9 (MMP9) as one of the proteins secreted in response to stress. Using cellular assays and in vivo microdialysis, we further find that stress-enhanced MMP9 secretion increases the cleavage of pro-brain-derived neurotrophic factor (proBDNF) to its mature form (mBDNF). BDNF is essential for adult synaptic plasticity and its pathway is associated with major depression and posttraumatic stress disorder. These findings unravel a cellular stress adaptation mechanism that bears the potential of opening avenues for the understanding of the pathophysiology of stress-related disorders.
The photocatalytic CO2 reduction reaction (CRR) represents a promising route for the clean utilization of stranded renewable resources, but poor selectivity resulting from the competing hydrogen ...evolution reaction (HER) in aqueous solution limits its practical applicability. In the present contribution a photocatalyst with hydrophobic surfaces was fabricated. It facilitates an efficient three‐phase contact of CO2 (gas), H2O (liquid), and catalyst (solid). Thus, concentrated CO2 molecules in the gas phase contact the catalyst surface directly, and can overcome the mass‐transfer limitations of CO2, inhibit the HER because of lowering proton contacts, and overall enhance the CRR. Even when loaded with platinum nanoparticles, one of the most efficient HER promotion cocatalysts, the three‐phase photocatalyst maintains a selectivity of 87.9 %. Overall, three‐phase photocatalysis provides a general and reliable method to enhance the competitiveness of the CRR.
A photocatalytic CO2 reduction reaction (CRR) in aqueous solution is a promising reaction route, while severe H2 generation (HER) greatly limits its selectivity and activity. A strategy to obtain a three‐phase contact of CO2 (gas), H2O (liquid) and catalyst (solid) is described to overcome the mass transfer limitation of CO2, elevate the CO2 concentration on the catalyst surface, restrain the HER, and enhance the activity and selectivity of the CRR.
More than 3000 clinical trials are evaluating the clinical activity of the PD-1 checkpoint inhibitors as monotherapies and in combinations with other cancer therapies 1. The PD-1 checkpoint ...inhibitors are remarkable for their clinical activities in shrinking tumors across a wide range of tumor types, in causing durable responses, and in their tolerability. These attributes position them as favorable agents in clinical combinations. Historically, approaches to cancer therapy combinations focused on agents with orthogonal activities to avoid shared resistance mechanisms and shared toxicities. Although CTLA-4/PD-1 combinations have progressed based on possible immune interactions, additional approaches have used more orthogonal treatments such as standard of care chemotherapies and anti-angiogenesis inhibitors. Using the concept of independent activity pioneered by Bliss 2, examples of these approaches were compared. Both standard of care chemotherapy and anti-angiogenesis combinations show promising clinical activity above that predicted by the independent contributions of the agents tested on their own. In contrast, the combinations of CTLA4/PD-1 checkpoint inhibitors in renal cancer and melanoma show no more activity than that predicted by the independent contributions of the monotherapies. This update on approaches to the development of clinical combination therapies highlights the potential importance of combining PD-1 checkpoint inhibitors with a broad range of clinically active partners.
Polysaccharides have attracted considerable attention in a broad range of applications in recent years, which is due to their remarkable features such as biocompatibility, biodegradability, renewable ...origin, and facile modification. Considerable research efforts have been focused on developing polysaccharide nanoparticles and to promote their applications in various areas and biomedicine in particular. The present review highlights the properties of common polysaccharides used in nanoparticle formation as well as strategies to fabricate polysaccharide nanoparticles. Furthermore, the combination of polysaccharide nanoparticles and polymers is presented and brought into the context of applications. Finally, applications of polysaccharide nanoparticles as nano-delivery system, Pickering emulsion stabilisers, and material reinforcing agent in the fields of nanomedicine, cosmetics, and food system are highlighted. Moreover, this review describes and critically discusses present limitations and drawbacks in the preparation and use of polysaccharide nanoparticles, revealing directions to develop polysaccharide nanoparticles for further utilisation in various applications in the future.
The present review highlights the developments in polysaccharide nanoparticles with a particular focus on applications in biomedicine, cosmetics and food.
A facile route to synthesize hydrophilically or hydrophobically grafted graphitic carbon nitride (g-CN) is reported. For this purpose, functionalized olefinic molecules with a low polymerization ...tendency are utilized for grafting onto the surface to preserve the features of g-CN while improving its dispersibility. One-pot, visible light-induced grafting yields highly dispersible g-CNs either in aqueous or organic media. Moreover, functional groups such as amines can be introduced, which yields pH-dependent dispersibility in aqueous media. Compared with unfunctionalized g-CN, low sonication times are sufficient to redisperse g-CN. In addition, because of increased dispersion stability, higher amounts of functionalized g-CN can be dispersed (up to 10% in aqueous dispersion and 2% in organic dispersion) when compared to unfunctionalized g-CN.
Microglia are the CNS resident immune cells that react to misfolded proteins through pattern recognition receptor ligation and activation of inflammatory pathways. Here, we studied how microglia ...handle and cope with α-synuclein (α-syn) fibrils and their clearance. We found that microglia exposed to α-syn establish a cellular network through the formation of F-actin-dependent intercellular connections, which transfer α-syn from overloaded microglia to neighboring naive microglia where the α-syn cargo got rapidly and effectively degraded. Lowering the α-syn burden attenuated the inflammatory profile of microglia and improved their survival. This degradation strategy was compromised in cells carrying the LRRK2 G2019S mutation. We confirmed the intercellular transfer of α-syn assemblies in microglia using organotypic slice cultures, 2-photon microscopy, and neuropathology of patients. Together, these data identify a mechanism by which microglia create an “on-demand” functional network in order to improve pathogenic α-syn clearance.
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•Microglia rapidly engulf exogenous α-synuclein but hesitate in its degradation•α-synuclein is transferred between microglia through tunneling nanotubes•Healthy microglia donate mitochondria to α-synuclein overloaded cells•Sharing the α-synuclein burden attenuated the inflammatory microglia profile
Microglia form F-actin dependent intercellular networks to transfer α-synuclein fibrils to neighboring microglial cells for degradation and clearance. Impairment in this process, as seen with Parkinson’s disease mutations, leads to increased inflammatory profiles and cell death.
A novel approach for a temperature-sensitive stabilization of water-in-water (W/W) emulsions is described. Specifically, we leveraged the thermal induced conformation change of tailored ...thermoresponsive block copolymers to reversibly stabilize and destabilize water-water interfaces. In addition, we investigated our approach to reversibly tune the reaction kinetics of enzymes compartmentalized within aqueous two-phase systems.
Temperature sensitive water-in-water (W/W) emulsions are described utilizing the thermal induced conformation change of tailored thermoresponsive block copolymers to reversibly stabilize and destabilize water-water interfaces.
Mesocrystalssuperstructures of crystalline nanoparticles that are aligned in a crystallographic fashionare of increasing interest for formation of inorganic materials with complex and sophisticated ...morphologies to tailor properties without changing chemical composition. Here we report morphogenesis of a novel mesocrystal consisting of nanoscale metal–organic frameworks (MOF) by using double hydrophilic block copolymer (DHBC) as a crystal modulator. DHBC selectively prefers the metastable hexagonal kinetic polymorph and promotes anisotropic crystal growth to generate hexagonal rod mesocrystals via oriented attachment and mesoscale assembly. The metastable nature of hexagonal mesocrystals enables further hierarchical morphogenesis by a solvent-mediated polymorphic transformation toward stable tetragonal mesocrystals that retain the outer hexagonal particle morphology. Furthermore, synthesis of hybrid MOFs, where hexagonal mesocrystals are vertically aligned on specific surfaces of cubic MOFs, is demonstrated. The present strategy opens a new avenue to create MOF mesocrystals and their hybrids with controlled size and morphology that can be designed for various potential applications.
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