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Chemistry. 2013 Aug 5;19(32):10543-50. doi: 10.1002/chem.201300864. Epub 2013 Jul 2.

Molecular-level insights into the oxidative degradation of grafted amines.

Author information

1
Department of Chemistry, Centre for Catalysis Research and Innovation, University of Ottawa, Ottawa, Ontario, K1N 6N5, Canada.

Abstract

The oxidative degradation of CO2 adsorbents consisting of amine-grafted pore-expanded mesoporous MCM-41 silica was investigated. The adsorbents were treated under flowing air at various temperatures, and the degree of deactivation was evaluated through the measurement of their CO2 adsorption capacity prior and subsequent to exposure to air. To decipher the chemical structure of surface species upon air-deactivation of grafted amines, a solvent extraction procedure was developed using a deuterated basic solution. The obtained solutions were analyzed by a variety of 1D and 2D NMR spectroscopy techniques, such as (29)Si, (13)C, (1)H, [(1)H,(15)N] HMBC, [(1)H,(13)C] HMQC, COSY and DOSY. The surface species generated by oxidative degradation of amine-grafted silica were found to contain functional groups such as imine, amide and carboxylic groups. Several structural units were conclusively demonstrated.

KEYWORDS:

adsorption; carbon dioxide; grafted amines; mesoporous materials; oxidative degradation

PMID:
23821582
DOI:
10.1002/chem.201300864

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