The precise control of mechanochemical activation within deep tissues via non-invasive ultrasound holds profound implications for advancing our understanding of fundamental biomedical sciences and revolutionizing disease treatments. However, a theory-guided mechanoresponsive materials system with well-defined ultrasound activation has yet to be explored. Here we present the concept of using porous hydrogen-bonded organic frameworks (HOFs) as toolkits for focused ultrasound programmably triggered drug activation to control specific cellular events in the deep brain, through on-demand scission of the supramolecular interactions.
View Article and Find Full Text PDFDeveloping adsorptive separation processes based on C H -selective sorbents to replace energy-intensive cryogenic distillation is a promising alternative for C H purification from C H /C H mixtures, which however remains challenging. During our studies on two isostructural metal-organic frameworks (Ni-MOF 1 and Ni-MOF 2), we found that Ni-MOF 2 exhibited significantly higher performance for C H /C H separation than Ni-MOF-1, as clearly established by gas sorption isotherms and breakthrough experiments. Density-Functional Theory (DFT) studies showed that the unblocked unique aromatic pore surfaces within Ni-MOF 2 induce more and stronger C-H⋅⋅⋅π with C H over C H while the suitable pore spaces enforce its high C H uptake capacity, featuring Ni-MOF 2 as one of the best porous materials for this very important gas separation.
View Article and Find Full Text PDFHighly efficient adsorptive separation of propylene from propane offers an ideal alternative method to replace the energy-intensive cryogenic distillation technology. Molecular sieving-type separation via high-performance adsorbents is targeted for superior selectivity, but the limit in adsorption capacity remains a great challenge. Here, we report an oxyfluoride-based ultramicroporous metal-organic framework , [Ni(WOF)(pyz)] (pyz = pyrazine), featuring one-dimensional pore channels that can accommodate the propylene molecules with optimal binding affinity while specifically excluding the propane molecules.
View Article and Find Full Text PDFA new rare earth based two-dimensional coordination network and a three-dimensional metal-organic framework (MOF) have been synthesized using bicinchoninic acid (BCA) and yttrium(iii) ions. Yttrium dimer nodes are formed in the absence of a modulator, resulting in a 2D layered coordination network (Y-BCA-2D). The presence of fluorinating agents, , 2-fluorobenzoic acid (2-FBA), 2,6-difluorobenzoic acid (2,6-DFBA), and perfluorohexanoic acid (PFHxA) result in μ-F bridged metal hexaclusters (YF) that form a three-dimensional MOF (Y-BCA-3D).
View Article and Find Full Text PDFPropylene is a crucial building block to produce many industrial-scale chemicals including polypropylene. The separation of propylene from propane to reach the high-purity levels needed for downstream applications is a difficult task due to the close similarities in their physical properties. The olefin/paraffin separation including that involving propylene mainly relies on highly energy-intensive distillation processes and accounts for nearly 0.
View Article and Find Full Text PDFSeparating carbon dioxide from fuel gases like hydrocarbons by physical adsorbents is industrially important and more energy-efficient than traditional liquid extraction or cryogenic distillation methods. It is very important while very challenging to develop CO -selective adsorbents, considering CO is less polarizable than light hydrocarbon molecules, particularly those simultaneously with almost identical molecular dimensions and physical properties, such as acetylene. Herein, an ultramicroporous metal-organic framework constructed from copper(II) and 5-fluoropyrimidin-2-olate, termed Cu-F-pymo, is carefully studied under different activations for inverse separation of CO from C H .
View Article and Find Full Text PDFThe quest for new and unique polynuclear metal-oxocarboxylate clusters has led to a continual boom of highly connected and robust metal-organic frameworks (MOFs) with intriguing properties. In this work, by virtue of a highly specific coordination-driven cluster rearrangement process of a presynthesized trinuclear zirconocene-based tripodal metallo-pyridine ligand, we realized the preparation of the first two 2D heterometallic MOFs incorporating unprecedented Johnson-type () nonanuclear Zr-oxocarboxylate clusters, as unambiguously uncovered by single-crystal X-ray crystallography. The resultant two charged frameworks feature counteranion-dependent 3,6-c kgd (JMOF-1) and 3,12-c 3,12L4 (JMOF-2) nets that are formed by octahedral and hexagonal prismatic Zr molecular building blocks (MBBs), respectively.
View Article and Find Full Text PDFHighly selective adsorptive separation of olefin/paraffin through porous materials can produce high purity olefins in a much more energy-efficient way than the traditional cryogenic distillation. Here we report an ultramicroporous cobalt gallate metal-organic framework (Co-gallate) for the highly selective sieving separation of propylene/propane at ambient conditions. This material possesses optimal pore structure for the exact confinement of propylene molecules while excluding the slightly large propane molecules, as clearly demonstrated in the neutron diffraction crystal structure of Co-gallate⊃0.
View Article and Find Full Text PDFCognitive impairment is a common complication of type 2 diabetes mellitus (T2DM) that may be related to iron deposition in the brain. Hepcidin is expressed in the brain and has the ability to regulate iron. Therefore, this study explored the role of hepcidin in hippocampal iron deposition and cognitive impairment in T2DM.
View Article and Find Full Text PDFGlioblastoma multiform (GBM) is the most lethal intracranial tumor in adults. Glioblastoma stem-like cells (GSCs) are responsible for tumorigenesis and chemotherapy resistance. BMPs are known to increase temozolomide (TMZ) response in GSCs, however, the intracellular molecular mechanism remains largely unknown.
View Article and Find Full Text PDFCarbon molecular sieve (CMS)-based membrane separation is a promising solution for hydrogen separation due to its great advantages on perm-selectivity, thermal stability, and chemical stability. To prepare high-performance CMS membranes, the molecular structure of polymer precursors and their arrangements should be primarily considered. In this work, a benzimidazole-based 6FDA (2,2'-bis(3,4'-dicarboxyphenyl) hexafluoropropane dianhydride)-type polyimide (PABZ-6FDA-PI) is chosen as precursor to prepare the CMS membrane.
View Article and Find Full Text PDFNeuropsychiatr Dis Treat
June 2020
Purpose: Impairments in intra- and inter-hemispheric information transfer circuits have been reported in patients with major depressive disorder (MDD). However, the specific anomalous connection (intra- and/or inter-hemispheric) and hemisphere (left and/or right) in which this connection plays a more dominant role in the pathogenic mechanism underlying MDD are still poorly understood.
Patients And Methods: Structural magnetic resonance imaging and resting-state functional magnetic resonance imaging were performed in 33 patients with MDD and 33 healthy controls.
Nanoscale metal-organic framework (nMOF) is a distinctive type of crystalline compounds that consists of metal ions or clusters coordinated to organic ligands. This hybrid material has attracted fast-growing attention due to its tunable pore sizes, remarkably large surface areas, and high selectivity in uptaking small molecules. In this paper, we successfully developed a novel approach for synthesizing a core-shell structure with MIL-88B-4CH as a tunable nMOF shell and MnFeO as a magnetic core.
View Article and Find Full Text PDFMimicking biological proton pumps to achieve stimuli-responsive protonic solids has long been of great interest for their diverse applications in fuel cells, chemical sensors, and bio-electronic devices. Now, dynamic light-responsive metal-organic framework hybrid membranes can be obtained by in situ encapsulation of photoactive molecules (sulfonated spiropyran, SSP), as the molecular valve, into the cavities of the host ZIF-8. The configuration of SSP can be changed and switched reversibly in response to light, generating different mobile acidic protons and thus high on/off photoswitchable proton conductivity in the hybrid membranes and device.
View Article and Find Full Text PDFThe present study investigated if c-MYC and high mobility group AT-hook 2 (HMGA2) expression was associated with prognosis of patients with pancreatic ductal adenocarcinoma (PDAC). A total of 102 patients undergoing surgery for PDAC were retrospectively reviewed. Immunohistochemistry was used to detect c-MYC and HMGA2 protein expression in PDAC and peritumoral tissue samples.
View Article and Find Full Text PDFUniform micron sized hierarchical COF (HCOF) spheres were fabricated by a template-free solution-based aging method at room temperature for the first time. The postsynthetic metalation of HCOF with Fe3+ makes the metalated HCOF an excellent photothermal agent (PTA) for photothermal therapy (PTT).
View Article and Find Full Text PDFLight-sensitive yolk-shell nanoparticles (YSNs) as remote-controlled and stimuli-responsive theranostic platforms provide an attractive method for synergistic cancer therapy. Herein, a kind of novel stimuli-responsive multifunctional YSNs has been successfully constructed by integrating star-shaped gold (Au star) nanoparticles as the second near-infrared (NIR-II) photothermal yolks and biodegradable crystalline zeolitic imidazolate framework-8 (ZIF-8) as the shells. In this platform, a chemotherapeutic drug (doxorubicin hydrochloride, DOX) was encapsulated into the cavity, which can show the behavior of controlled release due to the degradation process of ZIF-8 in the mildly acidic tumor microenvironment.
View Article and Find Full Text PDFPhotodynamic therapy (PDT) of cancers is usually inefficient due to the relatively low level of oxygen in cancer cells; therefore, it needs to combine with other treatment strategies such as chemotherapy or photothermal therapy (PTT) to achieve the best anticancer efficacy. Although porphyrin-containing materials have been widely studied for PDT, the photothermal effect is rarely reported. Herein, nanoscale porphyrin-containing covalent organic polymers (PCOPs) were produced via a room temperature solution-based aging method.
View Article and Find Full Text PDFPrevious studies have shown that type 2 diabetes mellitus (T2DM) can accelerate the rate of cognitive decline in patients. As an organ with high energy consumption, the brain network balances between lower energy consumption and higher information transmission efficiency. However, T2DM may modify the proportion of short- and long-range connections to adapt to the inadequate energy supply and to respond to various cognitive tasks under the energy pressure caused by homeostasis alterations in brain glucose metabolism.
View Article and Find Full Text PDFThe aim of this study was to investigate the relationship among left ventricular (LV) concentric hypertrophy, endocardial remodeling, and myocardial deformation in type-2 diabetes mellitus (T2DM). Fifty-three T2DM patients with normotension and 36 healthy controls underwent cardiovascular magnetic resonance imaging to assess for LV concentric hypertrophy (LV myocardial mass index, LVMMi; LVMMi-to-LV end-diastolic volume index ratio, MVR), endocardial remodeling (fractal dimension of trabeculations, FD), and myocardial deformation (global longitudinal, radial and circumferential strain, systolic and diastolic strain rate). When compared with healthy controls, T2DM was associated with LV concentric hypertrophy (LVMMi: T2DM, 52.
View Article and Find Full Text PDFIon-doped poly(p-phenylenediamine) (Fe-ppd) nanoparticles were prepared at room temperature by using FeCl3 as an oxidant. Fe-ppd exhibited high photothermal conversion efficiency (39.27%) and excellent photostability.
View Article and Find Full Text PDFTitanium dioxide (TiO ) has been widely investigated and used in many areas due to its high refractive index and ultraviolet light absorption, but the lack of absorption in the visible-near infrared (Vis-NIR) region limits its application. Herein, multifunctional Fe@γ-Fe O @H-TiO nanocomposites (NCs) with multilayer-structure are synthesized by one-step hydrogen reduction, which show remarkably improved magnetic and photoconversion effects as a promising generalists for photocatalysis, bioimaging, and photothermal therapy (PTT). Hydrogenation is used to turn white TiO in to hydrogenated TiO (H-TiO ), thus improving the absorption in the Vis-NIR region.
View Article and Find Full Text PDFSize- and shape-controlled growth of nanoscale microporous organic polymers (MOPs) is a big challenge scientists are confronted with; meanwhile, rendering these materials for in vivo biomedical applications is still scarce. In this study, a monodispersed nanometalated covalent organic polymer (MCOP, M=Fe, Gd) with sizes around 120 nm was prepared by a self-templated two-step solution-phase synthesis method. The metal ions (Fe , Gd ) played important roles in generating a small particle size and in the functionalization of the products during the reaction with p-phenylenediamine (Pa).
View Article and Find Full Text PDFGa-soc-MOF hollow cubes with an average size of about 300 nm were prepared by a polyvinylpyrrolidone (PVP) assisted acid etching process. Colloidosomes with sizes of around 5-10 μm composed of single-layer tetrakaidecahedron building blocks (BBs) were synthesized for the first time. Au@Ga-soc-MOF nanocomposites with excellent catalytic properties were obtained.
View Article and Find Full Text PDFPurpose: To study changes in the morphometric characteristics of the whole brain visual-related cortex in various stages of primary open angle glaucoma (POAG) in vivo.
Materials And Methods: Thirty POAG patients (nine early stage cases and 21 advanced-late stage cases) and 30 gender-, education-, and age-matched healthy controls were enrolled in the study. Image data were obtained with a T1 weighted three-dimensional magnetization prepared rapid acquisition gradient echo sequence (T1WI 3D MP RAGE).