FTIR Study of CO2 Adsorption on Amine-Grafted SBA-15: Elucidation of Adsorbed Species

被引:304
作者
Danon, Alon [1 ]
Stair, Peter C.
Weitz, Eric
机构
[1] Northwestern Univ, Inst Catalysis Energy Proc, Evanston, IL 60208 USA
关键词
CARBON-DIOXIDE; CARBAMIC ACID; SPECTROSCOPIC IDENTIFICATION; SILICA SURFACES; IR SPECTROSCOPY; REDUCTION; OXIDES; SITES;
D O I
10.1021/jp200914v
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The interaction between amines and CO2 offers a possible route for the catalytic activation of CO2. In situ infrared spectroscopy was used to study the interaction of CO2 with amine-grafted SBA-15. We employed three different types of amine-grafted SBA-15 surfaces to quantify the effect distinct tethered amine moieties have on the chemistry of CO, interacting with amine-grafted SBA-15. When the SBA-15 surface has a low density of amines and is "capped" to mitigate against interactions with surface-bound moieties, no new chemical species are observed on exposure to carbon dioxide. An ionic carbamate and a surface-bound carbamate are observed on the other SBA-15 surfaces on exposure to CO2. The formation of carbamates decreases the bond order of the carbon oxygen bond of the carbon dioxide molecule. The role of the different amine moieties and the surface silanol groups in the formation of the carbamates is discussed. Our results suggest that controlling the local environment around surface-grafted amines, which could be achieved by the use of suitably engineered surface environments, could facilitate the adsorption and activation of CO2.
引用
收藏
页码:11540 / 11549
页数:10
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