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Understanding the Reactivity of "Naked" Acyclic Carbene-like Species Featuring a Group 13 Element in the [4+1] Cycloaddition with Benzene.
Inorg Chem
January 2025
Department of Applied Chemistry, National Chiayi University, Chiayi 60004, Taiwan.
The chemical reactivity between benzene and the "naked" acyclic carbene-like (G13X) species, having two bulky N-heterocyclic boryloxy ligands at the Group 13 center, was theoretically assessed using density functional theory computations. Our theoretical studies show that (BX) preferentially undergoes C-H bond insertion with benzene, both kinetically and thermodynamically, whereas the (AlX) analogue favors a reversible [4 + 1] cycloaddition. Conversely, the heavier carbene analogues ((GaX), (InX), and (TlX)) are not expected to engage in a reaction with benzene.
View Article and Find Full Text PDFDo physical or imaging changes explain the effectiveness of progressive tendon loading exercises? A causal mediation analysis of athletes with patellar tendinopathy.
J Sci Med Sport
December 2024
Department of Orthopedics and Sports Medicine, Erasmus MC University Medical Center, the Netherlands.
Objectives: To investigate whether the effectiveness of progressive tendon loading exercises (PTLE) on patellar tendinopathy is mediated through changes in physical or imaging properties.
Design: Mediation analyses based on a randomized clinical trial (n = 76) in patellar tendinopathy comparing PTLE with eccentric exercise therapy (EET).
Methods: Pain-related disability on Victorian Institute of Sports Assessment-Patella (VISA-P, 0 to 100) and pain (Visual Analogue Score) after single-leg decline squat (VAS-SLDS, 0 to 10) at 24 weeks were outcome measures.
Tunability in Heterobimetallic Complexes Featuring an Acyclic "Tiara" Polyether Motif.
Inorg Chem
January 2025
Department of Chemistry, University of Kansas, 1567 Irving Hill Road, Lawrence, Kansas 66045, United States.
Both cyclic "crown" and acyclic "tiara" polyethers have been recognized as useful for the binding of metal cations and enabling the assembly of multimetallic complexes. However, the properties of heterobimetallic complexes built upon acyclic polyethers have received less attention than they deserve. Here, the synthesis and characterization of a family of eight redox-active heterobimetallic complexes that pair a nickel center with secondary redox-inactive cations (K, Na, Li, Sr, Ca, Zn, La, and Lu) bound in acyclic polyether "tiara" moieties are reported.
View Article and Find Full Text PDFIsochroman-3,4-dione and Tandem Aerobic Oxidation of 4-Bromoisochroman-3-one in the Highly Regio- and Diastereoselective Diels-Alder Reaction for the Construction of Bridged Polycyclic Lactones.
J Org Chem
December 2024
Dipartimento di Chimica e Biologia "A. Zambelli", Università degli Studi di Salerno, 84084 Fisciano, SA, Italy.
Herein we report two processes facilitated by diisopropylethylamine (DIPEA) for the synthesis of novel bridged polycyclic molecule analogues to natural products. The use of 4-bromoisochroman-3-one initiated an autoxidation reaction, followed by a Diels-Alder cycloaddition in the presence of electron-deficient dienophiles. Mechanistic studies revealed isochromane-3,4-dione as a key intermediate, which undergoes in situ dienolization/dearomatization followed by a [4 + 2] cycloaddition.
View Article and Find Full Text PDFDiphosphaenones: beyond the phosphorus analogue of enones.
Chem Sci
December 2024
LIFM, IGCME, School of Chemistry, Sun Yat-Sen University Guangzhou 510006 China
Phosphaenones, like their carbon analogue enones (C[double bond, length as m-dash]C-C[double bond, length as m-dash]O), are promising building blocks for synthetic chemistry and materials science. However, in contrast to the α- and β-phosphaenones, structurally and spectroscopically well-defined diphosphaenones (DPEs) are rare. In this study, we disclose the isolation and spectroscopic characterization of N-heterocyclic vinyl (NHV) substituted acyclic DPEs 3a,b [NHV-P[double bond, length as m-dash]P-C(O)-NHV].
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