Influence of Belousov-Zhabotinsky substrate concentrations on autonomous oscillation of polymer chains with Fe(bpy)3 catalyst

J Phys Chem B. 2014 Jun 19;118(24):6931-6. doi: 10.1021/jp500824e. Epub 2014 Jun 6.

Abstract

We studied the effect of initial substrate concentrations in the Belousov-Zhabotinsky (BZ) reaction on the optical transmittance self-oscillation behavior of a polymer chain consisting of N-isopropylacrylamide (NIPAAm) and a Fe catalyst ([Fe(bpy)3]). The driving force of this transmittance self-oscillation was the solubility difference between the reduced and oxidized states of the [Fe(bpy)3] moiety in the polymer chain. The amplitude of the soluble-insoluble self-oscillation of poly(NIPAAm-co-[Fe(bpy)3]) was significantly smaller than that of poly(NIPAAm-co-[Ru(bpy)3]). Theoretical simulation results attributed this behavior to the small difference in the solvent qualities, C*, of the reduced and oxidized states. Furthermore, we clarified that poly(NIPAAm-co-[Fe(bpy)3]) required a narrower concentration range of HNO3 to exhibit self-oscillation than poly(NIPAAm-co-[Ru(bpy)3]), since transmittance self-oscillation occurred only for [HNO3] = 0.3 M. The period of self-oscillation of poly(NIPAAm-co-[Fe(bpy)3]) in solution was controlled mainly by NaBrO3 concentration and was hardly influenced by the initial concentration of malonic acid.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • 2,2'-Dipyridyl / analogs & derivatives*
  • 2,2'-Dipyridyl / chemistry
  • Acrylic Resins / chemistry
  • Catalysis
  • Ferrous Compounds / chemistry*
  • Nitric Acid / chemistry
  • Organometallic Compounds / chemistry
  • Polymerization
  • Polymers / chemical synthesis
  • Polymers / chemistry*
  • Spectrophotometry

Substances

  • Acrylic Resins
  • Ferrous Compounds
  • Organometallic Compounds
  • Polymers
  • tris(2,2'-bipyridyl)ruthenium(II)
  • tris(2,2'-bipyridyl)-Fe(II) complex
  • poly-N-isopropylacrylamide
  • Nitric Acid
  • 2,2'-Dipyridyl