A Molecular Picture of the Adsorption of Glycine in Mesoporous Silica through NMR Experiments Combined with DFT-D Calculations

被引：60

作者：

Folliet, Nicolas ^{[1
,2
,3
]}

Gervais, Christel ^{[1
,2
]}

Costa, Dominique ^{[4
]}

Laurent, Guillaume ^{[1
,2
]}

Babonneau, Florence ^{[1
,2
]}

Stievano, Lorenzo ^{[5
]}

Lambert, Jean-Francois ^{[3
]}

Tielens, Frederik ^{[3
]}

机构：

[1] Univ Paris 06, F-75005 Paris, France

[2] Coll France, CNRS, Lab Chim Matiere Condensee Paris, F-75005 Paris, France

[3] Univ Paris 06, UMR 7197, Lab Reactivite Surface, F-94200 Ivry, France

[4] Ecole Natl Super Chim Paris, UMR 7045, Lab Physicochim Surfaces, F-75231 Paris, France

[5] Univ Montpellier 2, Equipe AIME, ICGM, UMR5253, F-34095 Montpellier 5, France

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2013年 / 117卷 / 08期

关键词：

SOLID-STATE NMR; DENSITY-FUNCTIONAL THEORY; SURFACE SILANOL SITES; AB-INITIO; AMINO-ACIDS; SILSESQUIOXANE MODELS; ZWITTERIONIC GLYCINE; MINERAL SURFACES; AMORPHOUS SILICA; INTERFACE;

D O I：

10.1021/jp312195a

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 adsorption behavior of the amino acid glycine in mesoporous silica has been investigated using a combination of quantum chemical calculations and NMR spectroscopy experiments. Glycine adsorption on two representative sites of an amorphous silica surface, vicinal silanols and a silanol nest, was investigated by DFT-D. The effect of water coadsorption on the energetics of adsorption and NMR shifts was characterized. It was found that the silanol nest is a more favorable site for glycine adsorption due to a local increased H-bond density. Co-adsorption with water is also favored, especially a water molecule between a SiOH and the ammonium moiety. NMR chemical shifts computed on these models fall into the observed C-13 and N-15 experimental range, suggesting that the presence of different energetically comparable adsorption configurations cannot be excluded.

引用

页码：4104 / 4114

页数：11

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