Herein we address the question of whether a supramolecular finite metal-organic structure such as a cage or metal-organic polyhedron (MOP) can be synthesized via controlled cleavage of a three-dimensional (3D) metal-organic structure. To demonstrate this, we report the synthesis of a Cu(II)-based cuboctahedral MOP through orthogonal olefinic bond cleavage of the cavities of a 3D, Cu(II)-based, metal-organic framework (MOF). Additionally, we demonstrate that controlling the ozonolysis conditions used for the cleavage enables Clip-off Chemistry synthesis of two cuboctahedral MOPs that differ by their external functionalization: one in which all 24 external groups represent a mixture of aldehydes, carboxylic acids, acetals and esters, and one in which all are aldehydes.
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http://dx.doi.org/10.1021/jacs.4c09431 | DOI Listing |
Mass Spectrom Rev
January 2025
Department of Chemistry, University of Texas at Austin, Austin, Texas, USA.
Mass spectrometry (MS) has become a critical tool in the characterization of covalently modified nucleic acids. Well-developed bottom-up approaches, where nucleic acids are digested with an endonuclease and the resulting oligonucleotides are separated before MS and MS/MS analysis, provide substantial insight into modified nucleotides in biological and synthetic nucleic. Top-down MS presents an alternative approach where the entire nucleic acid molecule is introduced to the mass spectrometer intact and then fragmented by MS/MS.
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, International Innovation Center for Forest Chemicals and Materials, College of Chemical Engineering, Nanjing Forestry University, Longpan Road 159, Nanjing 210037, China. Electronic address:
Glycerol is one of the most important biomass platform compounds that is a by-product of biodiesel production, and the selective cleavage of the CC bond of glycerol to produce liquid hydrogen carriers (i.e., formic acid and formaldehyde) offers a viable strategy to alleviate the currently faced energy shortages.
View Article and Find Full Text PDFChemSusChem
December 2024
National & Local Joint Engineering Research Center on Biomass Resource Utilization, College of Environmental Science and Engineering, Nankai University, Tianjin, 300350, P. R. China.
The cleavage and functionalization of carbon-carbon bonds are crucial for the reconstruction and upgrading of organic matrices, particularly in the valorization of biomass, plastics, and fossil resources. However, the inherent kinetic inertness and thermodynamic stability of C-C σ bonds make this process challenging. Herein, we fabricated a glucose-derived defect-rich hierarchical porous carbon as a heterogeneous catalyst for the oxidative cleavage and esterification of C(CO)-C bonds.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
KU Leuven: Katholieke Universiteit Leuven, Chemistry, BELGIUM.
Understanding the impact of oxidative modification on protein structure and functions is essential for developing therapeutic strategies to combat macromolecular damage and cell death. However, selectively inducing oxidative modifications in proteins remains challenging. Herein we demonstrate that [V6O13{(OCH2)3CCH2OH}2]2- (V6-OH) hybrid metal-oxo cluster can be used for selective protein oxidative cleavage and modifications.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
State Key Laboratory of Applied Organic Chemistry & College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China.
The cycloaddition of aziridines with unsaturated compounds is a valuable method for synthesizing nitrogen heterocycles. However, this process is predominantly substrate-controlled, posing significant challenges in regulating the regioselectivity of the C-N bond cleavage. In this study, we report a nickel-catalyzed dynamic kinetic activation strategy that enables catalyst-controlled activation of aziridines.
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