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Microheterogeneity in CH3OH/CD3OH mixture.

Władysław Wrzeszcz1, Sylwester Mazurek1, Roman Szostak1

  • 1Faculty of Chemistry, University of Wrocław, F. Joliot-Curie 14, 50-383 Wrocław, Poland.

Spectrochimica Acta. Part A, Molecular and Biomolecular Spectroscopy
|July 29, 2017
PubMed
Summary

This study shows that mixtures of methanol-d0 and methanol-d3 exhibit microheterogeneity, deviating slightly from ideal behavior due to isotopic effects in the methyl groups. The structure involves homoclusters and heteroclusters, with cyclic tetramers dominating.

Keywords:
2D correlation analysisATR-IRBinary mixturesChemometricsDFTExcess spectraHydrogen bondingLiquid phaseMCR-ALSMethanolMethanol‑d(3)MicroheterogeneityMolecular structureNIRSpectroscopy

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Area of Science:

  • Physical Chemistry
  • Chemical Physics
  • Molecular Spectroscopy

Background:

  • Microheterogeneity was previously observed in binary mixtures of unlike alcohols.
  • Isotopic substitution in the methyl group of methanol is theoretically predicted to influence OH group properties.

Purpose of the Study:

  • To investigate microheterogeneity in mixtures of very similar alcohols: methanol-d0 (CH3OH) and methanol-d3 (CD3OH).
  • To determine if isotopic substitution leads to molecular-level separation and deviation from ideal mixture behavior.

Main Methods:

  • Experimental analysis of CH3OH/CD3OH mixtures.
  • Theoretical calculations to support experimental findings.
  • Analysis of molecular structure, including homoclusters and heteroclusters.
  • Spectroscopic analysis of the 2ν(OH) band.

Main Results:

  • CH3OH/CD3OH mixtures deviate from ideal behavior, but to a lesser extent than mixtures of unlike alcohols.
  • Deviation primarily arises from differences between the CH3 and CD3 groups, with a minor contribution from OH groups.
  • Mixture structure comprises homoclusters and heteroclusters, similar to other alcohol mixtures.
  • Equimolar mixtures show the highest heterocluster population and deviation from ideal behavior.
  • Cyclic tetramers and larger clusters dominate the mixture structure, with negligible linear clusters.
  • Differences in the position and intensity of the 2ν(OH) band between CH3OH and CD3OH were observed despite similar hydrogen bonding.

Conclusions:

  • Isotopic substitution in methanol induces microheterogeneity and deviation from ideal mixture behavior.
  • The CH3/CD3 group difference is the main driver of this deviation.
  • The molecular structure is characterized by dominant cyclic clusters and a significant presence of both homoclusters and heteroclusters.