Carbamate Stabilities of Sterically Hindered Amines from Quantum Chemical Methods: Relevance ofr CO2 Capture

S. Gangarapu, A.T.M. Marcelis, H. Zuilhof

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22 Citations (Scopus)

Abstract

The influence of electronic and steric effects on the stabilities of carbamates formed from the reaction of CO2 with a wide range of alkanolamines was investigated by quantum chemical methods. For the calculations, B3LYP, M11-L, MP2, and spin-component-scaled MP2 (SCS-MP2) methods were used, coupled with SMD and SM8 solvation models. A reduction in carbamate stability leads to an increased CO2 absorption capacity of the amine and a reduction of the energy required for solvent regeneration. Important factors for the reduction of the carbamate stability were an increase in steric hindrance around the nitrogen atom, charge on the N atom and intramolecular hydrogen bond strength. The present study indicates that secondary ethanolamines with sterically hindering groups near the N atom show significant potential as candidates for industrial CO2-capture solvents.
Original languageEnglish
Pages (from-to)3936-3943
JournalChemPhysChem
Volume14
Issue number17
DOIs
Publication statusPublished - 2013

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Keywords

  • free-energy perturbations
  • carbon-dioxide
  • reaction-kinetics
  • aqueous-solutions
  • initio methods
  • absorption
  • 2-amino-2-methyl-1-propanol
  • methyldiethanolamine
  • monoethanolamine
  • technology

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