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2D Chiral Ag(I) Complexes with A-π-- and D-π--Type Dicarboxylic Acid Ligands: Presenting Significant Differences in Nonlinear Optical Responses.
Inorg Chem
January 2025
Henan Provincial Key Laboratory of Surface and Interface Science, Zhengzhou University of Light Industry, Zhengzhou 450002, P. R. China.
Three two-dimensional (2D) chiral Ag(I) complexes with formulas [Ag(L)(5-nipa)] (), [Ag(L)(5-nipa)] (), and {[Ag(L)(5-hipa)]·2HO} () were prepared through the reactions of AgO with enantiopure -monodentate N-donors (L/L) and different dicarboxylic acids bearing A (acceptor)-π-- and D (donor)-π--type structural features, where / = (-)/(+)-2-(4'-pyridyl)-4,5-pinene-pyridine, 5-Hnipa = 5-nitroisophthalic acid, and 5-Hhipa = 5-hydroxyisophthalic acid. A study of their nonlinear optical responses reveals that chiral and enantiomeric pairs with the A-π--type dicarboxylic acid ligand simultaneously display second- and third-harmonic generation (SHG and THG) responses, while chiral containing the D-π--type dicarboxylic acid ligand only exhibits a very strong THG response. The THG intensity of is 451 × α-SiO, being about 27 and 24 times larger than those of and , respectively.
View Article and Find Full Text PDFChiral Aldehyde/Palladium Catalysis Enables Asymmetric Branched-Selective Ring-Opening Functionalization of Methylenecyclopropanes with Amino Acid Esters.
J Am Chem Soc
January 2025
Key Laboratory of Applied Chemistry of Chongqing Municipality and Chongqing Key Laboratory of Soft-Matter Material Chemistry and Function Manufacturing, School of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, China.
Achieving catalytic asymmetric functionalization of methylenecyclopropanes (MCPs) by selective C-C bond cleavage is a notable challenge due to the intricate reaction partners involved. In this work, we report that chiral aldehyde/palladium combined catalysis enables the asymmetric functionalization of MCPs with NH-unprotected amino acid esters. This reaction proceeds through a regiospecific branched ring-opening mechanism, resulting in optically active α,α-disubstituted α-amino acid esters bearing nonconjugated terminal alkene units.
View Article and Find Full Text PDFAn expanded substrate scope for cross-chiral ligation enables efficient synthesis of long l-RNAs.
RSC Chem Biol
December 2024
Department of Chemistry, Texas A&M University College Station Texas 77843 USA
Despite the growing interest in mirror-image l-oligonucleotides, both as a robust nucleic acid analogue and as an artificial genetic polymer, their broader adoption in biochemical research and medicine remains hindered by challenges associated with the synthesis of long sequences, especially for l-RNA. Herein, we present a novel strategy for assembling long l-RNAs the joining of two or more shorter fragments using cross-chiral ligase ribozymes together with new substrate activation chemistry. We show that 5'-monophosphorylated l-RNA, which is readily prepared by solid-phase synthesis, can be activated by chemical attachment of a 5'-adenosine monophosphate (AMP) or diphosphate (ADP), yielding 5'-adenosyl(di- or tri-)phosphate l-RNA.
View Article and Find Full Text PDFMicro-corrugated chiral nematic cellulose nanocrystal films integrated with ionic conductive hydrogels leads to flexible materials for multidirectional strain sensing applications.
Int J Biol Macromol
January 2025
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, PR China. Electronic address:
Multidirectional strain sensors are of technological importance for wearable devices and soft robots. Here, we report that flexible materials capable of multidirectional anisotropic strain sensing can be constructed leveraging diffusion-induced infiltration of monomers and in situ polymerization of metal ion-containing double network hydrogels in and on the surface of micro-corrugated chiral nematic cellulose nanocrystal/glucose films. Integrating the micro-corrugated cellulose nanocrystal/glucose chiral nematic films with ionic conductive hydrogels of PAA-co-AAm/sodium alginate/Al endows the materials with multidirectional mechanoelectrical resistivity and mechanochromism anisotropy.
View Article and Find Full Text PDFBiaxially chiral compounds: research and development of synthesis.
Chem Commun (Camb)
January 2025
College of Chemistry, Central China Normal University, Wuhan 430079, Hubei, China.
With the rapid advancements in asymmetric catalysis, there is a growing need for the asymmetric selective synthesis of complex and diverse molecules with chiral axes. Axially chiral molecules are not only present in natural products and drugs but also in specialized chiral ligands and catalysts. The catalytic asymmetric synthesis of axially chiral molecules has garnered significant attention within the chemical community.
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