Metal-organic frameworks (MOFs) show remarkable potential in a broad array of applications given their physical and chemical versatility. Classical synthesis of MOFs is performed using solution chemistry at elevated temperatures to achieve reversible metal-ligand bond formation. These harsh conditions may not be suitable for chemical species sensitive to high temperature or prone to deleterious reactions with solvents. For instance, Pd(ii) is susceptible to reduction under solvothermal conditions and is not a common metal node of MOFs. We report a generic and facile mechanochemical strategy that directly incorporates a series of Pd(ii)-based heterobimetallic clusters into MOFs as metal nodes without Pd(ii) being reduced to Pd(0). Mechanochemistry features advantages of short reaction time, minimum solvent, high reaction yield, and high degree of synthetic control. Catalytic performances of lattice-confined heterobimetallic sites are examined for nitrene transfer reactions and we demonstrate that the chemoselectivity for allylic amination olefin aziridination is readily tuned by the identity of the first-row metal ion in Pd(ii)-based heterobimetallic clusters.
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http://dx.doi.org/10.1039/d4sc01918k | DOI Listing |
Polym Chem
August 2024
Department of Chemistry, The University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, USA.
While the conformational ensembles of disordered peptides and peptidomimetics are complex and challenging to characterize, they are a critical component in the paradigm connecting macromolecule sequence, structure, and function. In molecules that do not adopt a single predominant conformation, the conformational ensemble contains rich structural information that, if accessible, can provide a fundamental understanding related to desirable functions such as cell penetration of a therapeutic or the generation of tunable enzyme-mimetic architecture. To address the fundamental challenge of describing broad conformational ensembles, we developed a model system of peptidomimetics comprised of polar glycine and hydrophobic -butylglycine to characterize using a suite of analytical techniques.
View Article and Find Full Text PDFCarbohydr Polym
March 2025
Shanghai Key Laboratory of Regulatory Biology, School of Life Sciences, East China Normal University, Shanghai 200241, PR China. Electronic address:
Cellulose foams are renewable and biodegradable materials that are promising substitutes for plastic foams. However, the scale-up fabrication of cellulose foams is severely hindered by technological complexity and cost- and time-consuming drying processes. Here, we developed a facile and robust method to fabricate cellulose foams via oven-drying following surfactant-assisted mechanical foaming of cellulose nanofibers (CNFs).
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
School of Mechanical Engineering, Chengdu University, Chengdu, Sichuan 610106, China.
Electrochemical nitrite (NO) is a promising technology for NO removal and a sustainable method for generating valuable ammonia (NH), but this process is intricate and generates other byproducts. In this work, we propose a facile and low-cost method for the preparation of a CuMoO nanosheet array, which can serve as an efficient electrocatalyst for the reduction of NO to NH. The morphology of CuMoO can be adjusted by controlling the synthesis conditions.
View Article and Find Full Text PDFChemSusChem
January 2025
Griffith University, School of Engineering and Built Environment, 170 Kessels Rd, 4111, Nathan, AUSTRALIA.
Carbon dots (CDs) as a new class of photoluminescent zero-dimension carbon nanoparticles have attracted significant research interests owing to their extraordinary opto-electro-properties and biocompatibility. So far, almost all syntheses of CDs require either heat treatment or exertion of high energy fields. Herein, a scalable room-temperature vortex fluidic method is introduced to the CDs synthesis using the angled vortex fluidic device (VFD).
View Article and Find Full Text PDFSmall
January 2025
School of Chemical and Environmental Engineering, Shanghai Institute of Technology, 100 Haiquan Road, Shanghai, 201418, China.
How to improve the stability and activity of metal-organic frameworks is an attractive but challenging task in energy conversion and pollutant degradation of metal-organic framework materials. In this paper, a facile method is developed by fabricating titanium dioxide nanoparticles (TiO NPs) layer on 2D copper tetracarboxylphenyl-metalloporphyrin metal-organic frameworks with zinc ions as the linkers (ZnTCuMT-X, "Zn" represented zinc ions as the linkers, the first "T" represented tetracarboxylphenyl-metalloporphyrin (TCPP), "Cu" represented the Cu coordinated into the porphyrin macrocycle, "M" represented metal-organic frameworks, the second "T" represented TiO NPs layer, and "X" represented the added volume of n-tetrabutyl titanate (X = 100, 200, 300 or 400)). It is found that the optimized ZnTCuMT-200 showed greatly and stably enhanced H generation, which is ≈28.
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