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Impact of solvents and surfactants on the self-assembly of nanostructured amine functionalized silica spheres for CO_(2) capture

查看全文 作　　者：Edith [1]Berger;Maximilian [1]W.Hahn;Thomas [2]Przybilla;Benjamin [2]Winter;Erdmann [2]Spiecker;Andreas [1]Jentys;Johannes [1]A.Lercher 高影响力作者 机构地区：[1]Department of Chemistry and Catalysis Research Center,Technische Universitat Munchen Lichtenbergstraβe 4,85747 Garching,Germany;[2]Center for Nanoanalysis and Electron Microscopy(CENEM)&Institute of Micro-and Nanostructure Research,Friedrich-Alexander-Universitat Erlangen-Nurnberg,Cauerstraβe 6,91058 Erlangen,Germany高影响力机构 出　　处：《Journal of Energy Chemistry》索引2016年第25卷第2期,共9页高影响力期刊 基　　金：supported by the German Research Council(DFG)within the priority program(Schwerpunktprogramm),“Poröse Medien mit definierter Porenstruktur in der Verfahrenstechnik–Modellierung,Anwendngen,Synthese”(SPP 1570)under the projects LE 1187/10 and SP 648/4;the framework of the DFG Excellence Initiative the Cluster of Excellence“Engineering of Advanced Materials”(DFG EXC 415);funding via the DFG research training group GRK 1896 摘　　要：Macroscopic SiO_2 spheres with a homogeneous amine distribution were synthesized by a one-step emulsion based synthesis approach in a flow column reactor. The CO_2 adsorption capacity of the nanostructured amine-functionalized silica spheres was studied in absence and presence of H_2O. The structural properties were adjusted by varying solvents and surfactants during the synthesis and, at constant amine loadings, were found to be the main factor for influencing the CO_2 sorption capacities. Under water-free conditions CO_2 is bound to the amino groups via the formation of carbamates, which require two neighboring amino groups to adsorb one CO_2 molecule. At constant amine concentrations sorbents with lower surface area allow to establish a higher amine density on the surface, which enhances the CO_2 uptake capacities under dry conditions. In presence of H_2O the CO_2 adsorption changes to 1:1 stoichiometry due to stabilization of carbamates by protonation of H_2O and formation of further species such as bicarbonates, which should in principle double the adsorption capacities. Low concentrations of physisorbed H2O(0.3 mmol/g) did not impair the adsorption capacity of the adsorbents for CO_2, while at higher water uptakes(0.6 and 1.1 mmol/g) the CO_2 uptake is reduced, which could be attributed to capillary condensation of H_2O or formation of bulky reaction products blocking inner pores and access to active sites. 关 键 词：Carbon dioxide AMINES Green solvent SURFACTANT Water(H_(2)O) CARBAMATE BICARBONATE
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