期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 19, 期 32, 页码 10543-10550出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201300864
关键词
adsorption; carbon dioxide; grafted amines; mesoporous materials; oxidative degradation
资金
- Natural Sciences and Engineering Council of Canada (NSERC)
- Carbon Management Canada (CMC)
- Federal Government for the Canada Research Chair in Nanostructured Materials for Catalysis and Separation [20012015]
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 Si-29, C-13, H-1, [H-1, N-15] HMBC, [H-1, C-13] 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.
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