A series of hybrid hydrogels of poly(ethylene glycol) (PEG) were synthesized using gelatin as a crosslinker and investigated for controlled delivery of the first-generation cephalosporin antibiotic, Cefazedone sodium (CFD). A commercially available 4-arm-PEG-OH was first modified to obtain four-arm-PEG-succinimidyl glutarate (4-arm-PEG-SG), which formed the gelatin-PEG composite hydrogels (SN) through crosslinking with gelatin. To regulate the drug delivery, SN hydrogels with various solid contents and crosslinking degrees were prepared.
View Article and Find Full Text PDFIn view of the flue gas characteristics of cement kilns in China, the development of low-temperature denitrification catalysts with excellent anti-poisoning performance has important theoretical and practical significance. In this work, a series of MnCeO@TiO and tourmaline-containing MnCeO@TiO-T catalysts was prepared using a chemical pre-deposition method. It was found that the MnCeO@TiO-T2 catalyst (containing 2% tourmaline) exhibited the best low-temperature NH-selective catalytic reduction (NH-SCR) performance, yielding 100% NO conversion at 110 °C and above.
View Article and Find Full Text PDFRadioiodine (mainly I and I) is known to be dangerous nuclear waste due to its high toxicity, fast mobility and long radioactive half-life. As an emerging class of novel porous organic polymers, covalent organic frameworks (COFs) have demonstrated tremendous application potential in the field of radioactive iodine capture because of their high specific surface area and tunable pore structure. Herein, three π-conjugated pyrene-based COFs, namely PyTTA-BPDA-COF, PyTTA-BPY-COF, and PyTTA-BT-COF, have been successfully prepared and used as highly efficient adsorbents for iodine capture.
View Article and Find Full Text PDFCarbon dioxide (CO) coupled with epoxide to generate cyclic carbonate stands out in carbon neutrality due to its 100% atom utilization. In this work, the mechanism of CO cycloaddition with propylene oxide (PO) cocatalyzed by windmill-shaped polyoxovanadate, [(CNH)(CHO)VVO]·4CHOH (V-1), and -BuNX (X = Br, I) was thoroughly investigated using density functional theory (DFT) calculations. The ring-opening, CO-insertion, and ring-closing steps of the process were extensively studied.
View Article and Find Full Text PDFJ Colloid Interface Sci
November 2024
Photodynamic therapy (PDT) is an emerging treatment but often restricted by the availability of oxygen. Enhancing the lifespan of singlet oxygen (O) by fractionated generation is an effective approach to improve the efficacy of PDT. Herein, an imine-based nanoscale COF (TpDa-COF) has been synthesized and functionalized with a pyridone-derived structure (Py) to create a O-storing nanoplatform TpDa-COF@Py, which can reversibly capture and release O.
View Article and Find Full Text PDFThe design and synthesis of organic photocatalysts remain a great challenge due to their strict structural constraints. However, this could be mitigated by achieving structural flexibility by constructing permanent porosity into the materials. Conjugated microporous polymers (CMPs) are an emerging class of porous materials with an amorphous, three-dimensional network structure, which makes it possible to integrate the elaborate functional groups to enhance photocatalytic performance.
View Article and Find Full Text PDFAltern Ther Health Med
September 2024
Objective: China has an aging society; the issue of aging is becoming increasingly serious. This study aimed to explore the factors influencing the demand for medical treatment and health care services among the elderly and offer countermeasures and suggestions.
Methods: In this cross-sectional study, a questionnaire method was used to inquire about 386 elderly people in three communities from Bincheng District, Binzhou City, and Shandong Province.
ACS Appl Mater Interfaces
October 2023
Radioactive iodine from nuclear waste poses a huge threat to public safety and raises concerns about environmental pollution. There is thus a growing demand for developing novel adsorbents for highly effective iodine capture. In this work, we design and synthesize three novel conjugated microporous polymers, namely, TPE-PyTTA-CMP, TPE-TAPP-CMP, and TPE-TPDA-CMP, which are constructed by an imidization reaction based on octet and tetratopic linkers.
View Article and Find Full Text PDFPolyoxometalates (POMs) have a broad array of applied platforms with well-characterized catalysis to achieve N-H bond activation. Herein, the mechanism of the Anderson-type POM-based catalyst [FeMoO{(OCH)CNH}] ([TrisFeMoO], Tris = {(OCH)CNH}) for the N-H bond activation of hydrazine (PhHNNHPh) was investigated by density functional theory calculations. The results reveal that [TrisFeMoO] as the active species is responsible for the continuous abstraction of two electrons and two protons of PhHNNHPh via a proton-coupled electron transfer pathway, resulting in the activation of two N-H bonds in PhHNNHPh and thus the product PhNNPh.
View Article and Find Full Text PDFPrecise control of the structure and spatial distance of Lewis acid (LA) and Lewis base (LB) sites in a porous system to construct efficient solid frustrated Lewis pair (FLP) catalyst is vital for industrial application but remains challenging. Herein, we constructed FLP sites in a polyoxometalate (POM)-based metal-organic framework (MOF) by introducing coordination-defect metal nodes (LA) and surface-basic POM with abundant oxygen (LB). The well-defined and unique spatial conformation of the defective POM-based MOF ensure that the distance between LA and LB is at ~4.
View Article and Find Full Text PDFInjury to the anterior talofibular ligament (ATFL) is a common acute injury of the lateral foot ligament. Untimely and improper treatment significantly affects the quality of life and rehabilitation progress of patients. The purpose of this paper is to review the anatomy and the current methods of diagnosis and treatment of acute injury to the ATFL.
View Article and Find Full Text PDFBackground: Lung cancer is the most common cancer-related death worldwide. In 2022, the number of daily deaths of lung cancer was estimated to reach around 350 in the United States. Lung adenocarcinoma is the main subtype of lung cancer and patients with malignant pleural effusion (MPE) suffer from poor prognosis.
View Article and Find Full Text PDFCovalent organic frameworks (COFs) hold the potential in converting CO with water into value-added fuels and O to save the deteriorating ecological environment. However, reaching high yield and selectivity is a grand challenge under metal-, photosensitizer-, or sacrificial reagent-free conditions. Here, inspired by microstructures of natural leaves, we designed triazine-based COF membranes with the integration of steady light-harvesting sites, efficient catalytic center, and fast charge/mass transfer configuration to fabricate a novel artificial leaf for the first time.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
May 2023
Metal-nitrogen-carbon catalysts, as promising alternative to platinum-based catalysts for oxygen reduction reaction (ORR), are still highly expected to achieve better performance by modulating the composition and spatial structure of active site. Herein, we constructed the non-planar nest-like [Fe S ] cluster sites in N-doped carbon plane. Adjacent double Fe atoms effectively weaken the O-O bond by forming a peroxide bridge-like adsorption configuration, and the introduction of S atoms breaks the planar coordination of Fe resulting in greater structural deformation tension, lower spin state, and downward shifted Fe d-band center, which together facilitate the release of OH* intermediate.
View Article and Find Full Text PDFAchalasia cardia, type of esophageal dynamic disorder, is a relatively rare primary motor esophageal disease characterized by the functional loss of plexus ganglion cells in the distal esophagus and lower esophageal sphincter. Loss of function of the distal and lower esophageal sphincter ganglion cells is the main cause of achalasia cardia, and is more likely to occur in the elderly. Histological changes in the esophageal mucosa are considered pathogenic; however, studies have found that inflammation and genetic changes at the molecular level may also cause achalasia cardia, resulting in dysphagia, reflux, aspiration, retrosternal pain, and weight loss.
View Article and Find Full Text PDFCobalt coordinated covalent organic frameworks have attracted increasing interest in the field of CO photoreduction to CO, owing to their high electron affinity and predesigned structures. However, achieving high conversion efficiency is challenging since most Co related coordination environments facilitate fast recombination of photogenerated electron-hole pairs. Here, we design two kinds of Co-COF catalysts with oxygen coordinated Co atoms and find that after tuning of coordination environment, the reported Co framework catalyst with Co-O sites exhibits a high CO production rate of 18000 µmol g h with selectivity as high as 95.
View Article and Find Full Text PDFHighly efficient removal of Hg(ii) has been previously achieved through the adsorption by functionalized covalent organic frameworks (COFs). Among these COFs, thioether groups need to be deliberately introduced into the pores of COFs through either a bottom-up synthesis or post-synthesis strategy. Herein, we report a simple mercury removal strategy that used a stable alkynyl (-C[triple bond, length as m-dash]C-) based covalent organic framework (TP-EDDA COF) as an adsorbent for Hg(ii) removal.
View Article and Find Full Text PDFTransforming CO into value-added chemicals has been an important subject in recent years. The development of a novel heterogeneous catalyst for highly effective CO conversion still remains a great challenge. As an emerging class of porous organic polymers, covalent organic frameworks (COFs) have exhibited superior potential as catalysts for various chemical reactions, due to their unique structure and properties.
View Article and Find Full Text PDFAs one of the main nuclear wastes generated in the process of nuclear fission, radioactive iodine has attracted worldwide attention due to its harm to public safety and environmental pollution. Therefore, it is of crucial importance to develop materials that can rapidly and efficiently capture radioactive iodine. Herein, we report the construction of three electron-rich porous organic polymers (POPs), denoted as POP-E, POP-T and POP-P via Schiff base polycondensations reactions between -symmetric adamantane knot and four-branched "linkage" molecules.
View Article and Find Full Text PDFCovalent organic frameworks (COFs) are an emerging class of crystalline porous polymers that make these materials suitable for use as excellent scaffold in heterogeneous catalysis. Here we synthesize a layered two-dimensional (2D) COF (TADP-COF) through the condensation reaction between four-branched 5,10,15,20-tetrakis(4-aminophenyl)porphyrin (TAPP) and linear 2,5-dihydroxyterephthalaldehyde (Dha) and 1,4-phthalaldehyde (PA) building blocks. Porphyrin units, imine and hydroxyl groups together with imines can provide wide coordination sites for metal docking.
View Article and Find Full Text PDFIn this work, the mechanism of water oxidation catalyzed by an Ru-based complex [Ru(L)] (L = 5,5-chelated 2-carboxyl-phen, 2,2';6',2''-terpyridine) was studied by density functional theory (DFT) calculations. In [Ru(L)], a carboxyl group is included in the second coordination sphere and plays an important role in the catalytic process. In the oxidation activation stage of water oxidation catalysis, the carboxyl group is proposed as a promising proton acceptor to promote proton transfer, which results in active Ru[double bond, length as m-dash]O species.
View Article and Find Full Text PDFThe design and synthesis of polynuclear metal cluster-based coordination cages is of considerable interest due to their appealing structural characteristics and potential applications. Herein, we report a calix[4]resorcinarene-based [Co] coordination cage, [Co(TPC4R-I)(1,3-BDC)(μ-OH)(HO)(DMF)]·7DMF·23HO (), assembled with 2 bowl-shaped calix[4]resorcinarenes (TPC4R-I), 10 angular 1,3-benzenedicarboxylates (1,3-BDC), and 12 Co(II) cations. Remarkably, it is shown to be a highly efficient recyclable heterogeneous catalyst for CO conversion due to its exposed Co(II) Lewis acid sites.
View Article and Find Full Text PDFThe performance of Mn-monosubstituted heteropolytungstates [Mn(HO)GeWO] ([GT-Mn-OH], where GT = GeWO) and [Mn(HO)GeWO] ([GT-Mn-OH]) as water oxidation catalysts at pH 9 was explored using density functional theory calculations. The counterion effect was fully considered, in which five and six Na ions were included in the calculations for water oxidation catalyzed by [GT-Mn-OH] and [GT-Mn-OH], respectively. The process of water oxidation catalysis was divided into three elemental stages: (i) oxidative activation, (ii) O-O bond formation, and (iii) O evolution.
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