Dithiophosphoric acids (DTPAs) are an intriguing class of compounds that are sourced from elemental sulfur and white phosphorus and are prepared from the reaction of phosphorus pentasulfide with alcohols. The electrophilic addition of DTPAs to alkenes and unsaturated olefinic substrates is a known reaction, but has not been applied to polymer synthesis and polymer functionalization. We report on the synthesis and application of DTPAs for the functionalization of challenging poly-enes, namely polyisoprene (PI) and polynorbornene (pNB) prepared by ring-opening metathesis polymerization (ROMP). The high heteroatom content within DTPA moieties impart intriguing bulk properties to poly-ene materials after direct electrophilic addition reactions to the polymer backbone introducing DTPAs as side chain groups. The resulting materials possess both enhanced optical and flame retardant properties vs the poly-ene starting materials. Finally, we demonstrate the ability to prepare crosslinked polydiene films with di-functional DTPAs, where the crosslinking density and thermomechanical properties can be directly tuned by DTPA feed ratios.
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http://dx.doi.org/10.1002/anie.202315963 | DOI Listing |
Org Biomol Chem
November 2024
Department of Pharmacy, Nanyang Medical College, Nanyang 473061, China.
Here, a photocatalytic three-component reaction between arylalkenes, quinoxalinones and dialkyl dithiophosphoric acids was developed. This protocol allows the simultaneous incorporation of heterocyclic and dithiophosphoryl groups into a single molecule structure efficiently. These functionalities are important precursors in medicinal chemistry.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2024
Department of Chemistry and Biochemistry, The University of Arizona, Tucson, AZ 85721, USA.
Dithiophosphoric acids (DTPAs) are an intriguing class of compounds that are sourced from elemental sulfur and white phosphorus and are prepared from the reaction of phosphorus pentasulfide with alcohols. The electrophilic addition of DTPAs to alkenes and unsaturated olefinic substrates is a known reaction, but has not been applied to polymer synthesis and polymer functionalization. We report on the synthesis and application of DTPAs for the functionalization of challenging poly-enes, namely polyisoprene (PI) and polynorbornene (pNB) prepared by ring-opening metathesis polymerization (ROMP).
View Article and Find Full Text PDFJ Org Chem
February 2022
School of Chemistry and Molecular Biosciences, The University of Queensland, St. Lucia, QLD 4072, Australia.
Quantum chemical calculations have successfully predicted the stereoselectivities of many BINOL phosphoric acid catalyzed reactions over the past 10-15 years. Herein we report a contrasting example: a reaction for which standard quantum chemistry techniques have proven unexpectedly ineffective at explaining the stereoselectivity. The Nazarov cyclizations of a divinyl ketone catalyzed by a BINOL phosphoric acid or H-BINOL dithiophosphoric acid were studied with a conventional contemporary quantum chemical approach, consisting of transition state optimizations with B3LYP-D3(BJ) and single-point calculations with several functionals in implicit solvent.
View Article and Find Full Text PDFBioorg Med Chem
January 2019
Institute of Fundamental Medicine and Biology, Kazan (Volga Region) Federal University, 420008 Kazan, 18 Kremlyovskaya St., Russia. Electronic address:
The pyridine-derived biomolecules are of considerable interest in developing medicinal compounds with various specific activities. Novel ammonium salts of pyridoxine, (S)-(-)-nicotine and nicotinamide with O,O-diorganyl dithiophosphoric acids (DTPA) were synthesized and characterized. The complexation of chiral monoterpenyl DTPA, including (S)-(-)-menthyl, (R)-(+)-menthyl, (1R)-endo-(+)-fenchyl, (1S,2S,3S,5R)-(+)-isopinocampheolyl derivatives, with pyridoxine and nicotine provided effective antibacterial compounds 3a,b,e,f, and 5a,b,d,f with MIC values against Gram-positive bacteria as low as 10 µM (6 µg/mL).
View Article and Find Full Text PDFPeptides
January 2018
Institute of Fundamental Medicine and Biology, Kazan (Volga Region) Federal University, 420008 Kazan, 18 Kremlyovskaya St., Russia. Electronic address:
Reactions of glutathione (GSH) with O,O-diorganyl dithiophosphoric acids (DTPA) were studied to develop bioactive derivatives of GSH. Effective coupling reaction of GSH with DTPA was proposed to produce the ammonium dithiophosphates (GSH-DTPA) between the NH group in γ-glutamyl residue of GSH and the SH group in DTPA. A series of the GSH-DTPA salts based on O-alkyl or O-monoterpenyl substituted DTPA were synthesized.
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