Relationships among pore size, connectivity, dimensionality of capillary condensation, and pore structure tortuosity of functionalized mesoporous silica

Armatas, GS; Salmas, CE; Louloudi, M; Androutsopoulos, GP; Pomonis, PJ

dc.contributor.author	Armatas, GS	en
dc.contributor.author	Salmas, CE	en
dc.contributor.author	Louloudi, M	en
dc.contributor.author	Androutsopoulos, GP	en
dc.contributor.author	Pomonis, PJ	en
dc.date.accessioned	2014-03-01T01:19:29Z
dc.date.available	2014-03-01T01:19:29Z
dc.date.issued	2003	en
dc.identifier.issn	0743-7463	en
dc.identifier.uri	https://dspace.lib.ntua.gr/xmlui/handle/123456789/15525
dc.subject	Pore Size	en
dc.subject	Pore Structure	en
dc.subject	Silica	en
dc.subject.classification	Chemistry, Physical	en
dc.subject.other	Adsorption isotherms	en
dc.subject.other	Ammonia	en
dc.subject.other	Condensation	en
dc.subject.other	Mesoporous materials	en
dc.subject.other	Pore size	en
dc.subject.other	Temperature programmed desorption	en
dc.subject.other	Thermodynamics	en
dc.subject.other	Pore structure tortuosity	en
dc.subject.other	Silica	en
dc.title	Relationships among pore size, connectivity, dimensionality of capillary condensation, and pore structure tortuosity of functionalized mesoporous silica	en
heal.type	journalArticle	en
heal.identifier.primary	10.1021/la020261h	en
heal.identifier.secondary	http://dx.doi.org/10.1021/la020261h	en
heal.language	English	en
heal.publicationDate	2003	en
heal.abstract	Seven mesoporous forms of silica were prepared by controlled and gradual functionalization of the original SiO2 surface with silano-(trimethoxy)-propyl-imidazole groups. The degree of surface functionalization was n = 0.00, 0.23, 0.30, 0.40, 0.52, 0.60, and 0.85 and was controlled by previous knowledge of surface acidity, determined by temperature-programmed desorption of NH3. From N-2 adsorption/desorption measurements, the specific surface area S-p (m(2) g(-1)), the specific pore volume VP (cm(3) g(-1)), and the corresponding pore size distributions (PSDs) were determined. The connectivity c of the solids was also calculated according to the method of Seaton, and the dimensionality of capillary condensation D-cc was found using the thermodynamic method of Neimark. The increase of functionalization. resulted in a linear drop of S-p and V-p, and the maximum D-max of the PSD and the full width at half-maximum, fwhm similar to2sigma, of the distribution drop in a regular way whereas the ratio (D-max/2sigma) remains practically constant. The connectivity c also decreases from c = 12.5 at n = 0 to c = 3 at n = 0.60-0.85, presumably because of blocking of channels connecting various pores. The D-cc values decrease with increasing n values. Next, the co-called corrugated pore structure model, CPSM, was employed for the estimation of tortuosity tau of the porous solids and the simulation of the experimental adsorption/desorption isotherms. From those CPSM simulations, the corresponding specific surface area S-CPSM (m(2) g(-1)), the specific pore volume V-CPSM (cm(3), g(-1)), and the corresponding pore size distribution PSDCPSM were estimated. The tortuosity tau of the system drops with the degree of functionalization from tau = 4.22 at n = 0 to tau = 3.37 at the initial functionalization (n = 0.23) and subsequently remains practically constant at about tau = 3.40 +/- 0.10, for the same reasons which affect the connectivity, that is, blocking ofvarious pore channels. The comparison between the parameters V-p and V-CPSM is quite satisfactory. The S-CPSM values appear systematically higher by 8-23% compared to the S-p ones. The dimensionality of capillary condensation D-cc is related to the variance 2sigma of the PSD. The reasons and the limits of this relationship are discussed.	en
heal.publisher	AMER CHEMICAL SOC	en
heal.journalName	Langmuir	en
dc.identifier.doi	10.1021/la020261h	en
dc.identifier.isi	ISI:000182389100009	en
dc.identifier.volume	19	en
dc.identifier.issue	8	en
dc.identifier.spage	3128	en
dc.identifier.epage	3136	en