Combined Experimental and Theoretical Study of the Competitive Absorption of CO2 and NO2 by a Superbase Ionic Liquid

Adam J. Greer, S. F. Rebecca Taylor, Helen Daly, Matthew G. Quesne, Nora H. de Leeuw, C. Richard A. Catlow, Johan Jacquemin, Christopher Hardacre

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Abstract

A superbase ionic liquid (IL), trihexyltetradecylphosphonium benzimidazolide ([P66614][Benzim]), is investigated for the capture of CO2 in the presence of NO2 impurities. The effect of the waste gas stream contaminant on the ability of the IL to absorb simultaneously CO2 is demonstrated using novel measurement techniques, including a mass spectrometry breakthrough method and in situ infrared spectroscopy. The findings show that the presence of an industrially relevant concentration of NO2 in a combined feed with CO2 has the effect of reducing the capacity of the IL to absorb CO2 efficiently by ∼60% after 10 absorption–desorption cycles. This finding is supported by physical property analysis (viscosity, 1H and 13C NMR, and X-ray photoelectron spectroscopy) and spectroscopic infrared characterization, in addition to density functional theory (DFT) calculations, to determine the structure of the IL-NO2 complex. The results are presented in comparison with another flue gas component, NO, demonstrating that the absorption of NO2 is more favorable, thereby hindering the ability of the IL to absorb CO2. Significantly, this work aids understanding of the effects that individual components of flue gas have on CO2 capture sorbents, through studying a contaminant that has received limited interest previously.
Original languageEnglish
Pages (from-to)7578-7586
Number of pages9
JournalACS Sustainable Chemistry & Engineering
Volume9
Issue number22
Early online date26 May 2021
DOIs
Publication statusPublished - 07 Jun 2021

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