FTIR Study of CO2 Adsorption on Amine-Grafted SBA-15: Elucidation of Adsorbed Species
FTIR Study of CO2 Adsorption on Amine-Grafted SBA-15: Elucidation of Adsorbed Species
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DOI：
10.1021/jp200914v
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发表时间：
2011-06-16
影响因子：
3.7
通讯作者：
Weitz, Eric
中科院分区：
文献类型：
--
作者：
Danon, Alon;Stair, Peter C.;Weitz, Eric
胺与CO2的相互作用为CO2的催化活化提供了一条可能的途径。采用原位红外光谱研究了CO2与胺接枝SBA-15的相互作用。我们采用了三种不同类型的胺接枝的SBA-15表面，以量化不同的拴系胺部分对CO的化学性质的影响，与胺接枝的SBA-15相互作用。当SBA-15表面具有低密度的胺并且被“封端”以减轻与表面结合部分的相互作用时，在暴露于二氧化碳时没有观察到新的化学物质。离子氨基甲酸酯和表面结合的氨基甲酸酯上观察到的其他SBA-15表面上暴露于CO2。氨基甲酸酯的形成降低了二氧化碳分子的碳氧键的键级。不同的胺部分和表面的硅烷醇基团在形成的氨基甲酸酯的作用进行了讨论。我们的研究结果表明，控制表面接枝胺周围的局部环境，这可以通过使用适当的工程表面环境来实现，可以促进CO2的吸附和活化。
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.