Temperature-Triggered Switchable Helix-Helix Inversion of Poly(phenylacetylene) Bearing l-Valine Ethyl Ester Pendants and Its Chiral Recognition Ability

Molecules. 2016 Nov 21;21(11):1583. doi: 10.3390/molecules21111583.

Abstract

A phenylacetylene containing the l-valine ethyl ester pendant (PAA-Val) was synthesized and polymerized by an organorhodium catalyst (Rh(nbd)BPh₄) to produce the corresponding one-handed helical cis-poly(phenylacetylene) (PPAA-Val). PPAA-Val showed a unique temperature-triggered switchable helix-sense in chloroform, while it was not observed in highly polar solvents, such as N,N'-dimethylformamide (DMF). By heating the solution of PPAA-Val in chloroform, the sign of the CD absorption became reversed, but recovered after cooling the solution to room temperature. Even after six cycles of the heating-cooling treatment, the helix sense of the PPAA-Val's backbone was still switchable without loss of the CD intensity. The PPAA-Val was then coated on silica gel particles to produce novel chiral stationary phases (CSPs) for high-performance liquid chromatography (HPLC). These novel PPAA-Val based CSPs showed a high chiral recognition ability for racemic mandelonitrile (α = 2.18) and racemic trans-N,N'-diphenylcyclohexane-1,2-dicarboxamide (α = 2.60). Additionally, the one-handed helical cis-polyene backbone of PPAA-Val was irreversibly destroyed to afford PPAA-Val-H by heating in dimethyl sulfoxide (DMSO) accompanied by the complete disappearance of the Cotton effect. Although PPAA-Val-H had the same l-valine ethyl ester pendants as its cis-isomer PPAA-Val, it showed no chiral recognition. It was concluded that the one-handed helical cis-polyene backbone of PPAA-Val plays an important role in the chiral recognition ability.

Keywords: chiral stationary phases; cis-to-trans isomerization; helical poly(phenylacetylene); helix-helix inversion; temperature-triggered.

MeSH terms

  • Acetylene / analogs & derivatives*
  • Acetylene / chemical synthesis
  • Acetylene / chemistry
  • Circular Dichroism
  • Ethyl Ethers / chemistry*
  • Molecular Conformation*
  • Photoelectron Spectroscopy
  • Polymerization
  • Proton Magnetic Resonance Spectroscopy
  • Stereoisomerism
  • Temperature*
  • Valine / chemistry*

Substances

  • Ethyl Ethers
  • poly(phenylacetylene)
  • Valine
  • Acetylene