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Recently, the correlation theory of the chemical bond was developed, which applies concepts of quantum information theory for the characterization of chemical bonds, based on the multiorbital correlations within the molecule. Here, for the first time, we extend the use of this mathematical toolbox for the description of electron-deficient bonds. We start by verifying the theory on the textbook example of a molecule with three-center two-electron bonds, namely, diborane(6). We then show that the correlation theory of the chemical bond is able to properly describe the bonding situation in more exotic molecules which have been synthesized and characterized only recently, in particular, the diborane molecule with four hydrogen atoms [diborane(4)] and a neutral zerovalent s-block beryllium complex, whose surprising stability was attributed to a strong three-center two-electron π bond stretching across the C-Be-C core. Our approach is of high importance especially in the light of a constant chase after novel compounds with extraordinary properties where the bonding is expected to be unusual.
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http://dx.doi.org/10.1063/1.5093497 | DOI Listing |
Angew Chem Int Ed Engl
September 2025
State Key Laboratory of Chemo and Biosensing, College of Chemistry and Chemical Engineering, Hunan University, Changsha, Hunan, 410082, P.R. China.
Organostibines exhibit significant potential as functional handles for the construction of C─C-rich scaffolds owing to their orthogonal and robust reactivity features. At present, the transformation of C(sp)/C(sp)─Sb bonds into C─C bonds has established a mature methodology. However, breakthroughs in the C(sp)─Sb system still require systematic investigations into reaction mechanisms, catalyst design, and other aspects.
View Article and Find Full Text PDFOrg Lett
September 2025
School of Pharmaceutical Sciences & Institute of Materia Medica, Medical Science and Technology Innovation Center, Shandong First Medical University & Shandong Academy of Medical Sciences, Jinan 250117, Shandong, P. R. China.
In this work, we developed nucleophilic 2-aminoallyl cations guided by DFT calculations. Computational insights enabled a comprehensive analysis of factors governing N-nucleophilicity and an accurate prediction of cycloaddition reactivity with electron-deficient alkenes. Notably, this study represents the first asymmetric [3 + 2] cycloaddition of amino-allyl cations with exocyclic double bonds, enabling the efficient synthesis of -pyrrolidines with excellent diastereoselectivities and enantioselectivities.
View Article and Find Full Text PDFACS Cent Sci
August 2025
Department of Nuclear Engineering, The Pennsylvania State University, University Park, Pennsylvania 16802, United States.
Two-dimensional (2D) nanomaterials are of great interest due to their unique properties and broad biological applications. Among these, borophene, a single-atom-thick boron sheet with a honeycomb structure, exhibits exceptional structural, electronic, and mechanical characteristics, making it a promising candidate for sensing, electronics, and biosensing. In this study, we report on a liquid-phase exfoliation method to synthesize stable borophene nanosheets and introduce a photoinduced immobilization technique to functionalize their surfaces with antibodies.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
Department of Chemistry and Shenzhen Grubbs Institute, Southern University of Science and Technology, Shenzhen, 518055, China.
The application of chalcogen bonding catalysis has been largely confined to benchmark reactions due to the limited structural diversity and activating ability of the catalysts, especially those derived from tellurium. Herein, we present a group of rationally designed bis-telluronium catalysts and realize the first application of chalcogen bonding donor in catalyzing the [4 + 2] cycloaddition reaction between azetidines and non-activated alkenes or alkynes. This chemistry demonstrates excellent functional group tolerance and offers an efficient avenue to access the piperidine and tetrahydropyridine architectures in generally moderate-to-good efficiency.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
Guangdong Provincial Key Laboratory of Fuel Cell Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou, 510640, China.
Metal-organic frameworks (MOFs) with well-defined crystalline structures offer ideal platforms to unravel structure-property relationships, but their low density of accessible metal sites limits catalytic activation. Efforts to generate open metal sites often compromise structural integrity, obstructing mechanistic investigation. In this study, we convert single-coordinated MOFs into dual-coordinated frameworks, enabling controlled creation of unsaturated metal sites to boost electrocatalytic performance while preserving crystal framework for structure-property study.
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