Chemically Modified Silica Materials as Model Systems for the Characterization of Water-Surface Interactions

Brodrecht, Martin; Kumari, Bharti; Breitzke, Hergen; Gutmann, Torsten; Buntkowsky, Gerd

doi:10.1515/zpch-2017-1059

Cited by 18 publications

(26 citation statements)

References 81 publications

(124 reference statements)

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“…There are two different strategies for obtaining such peptide-functionalized silica materials, namely an activation of the silica by virtue of a linker group, followed by a grafting of the previously synthesized peptide as shown, e.g., in [ 47 , 112 ] or the direct synthesis of the desired peptide inside the pores employing a modification of the standard SPPS protocol [ 176 , 177 , 194 ].…”

Section: Porous Host Materialsmentioning

confidence: 99%

“…To tackle this problem, 2 H NMR was used to investigate reorientation dynamics of unfreezable water (D 2 O) in MCM-41 and SBA-15 pores over wide temperature ranges towards the glass transition [ 45 , 176 , 181 , 183 , 213 , 214 , 215 , 216 , 217 , 218 , 219 ]. In particular, spin-lattice relaxation, line-shape analysis, and stimulated-echo experiments were combined to ensure broad dynamic ranges and the pore-size was systematically varied to study possible finite-size effects.…”

Section: Simple Liquids In Confinementmentioning

confidence: 99%

“…( d ): experimental variable temperature 2 H solid-echo NMR spectra of the melting process of naphthalene-d 8 inside MCM-41 (d aver = 33 Å) (i): experiment; (ii): simulated octahedral jump; (iii): two-phase model). All spectra are normalized to equal height (figure reproduced with permission from [ 176 ], copyright Walter de Gruyter and Company).…”

Section: Figurementioning

confidence: 99%

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Small Molecules, Non-Covalent Interactions, and Confinement

Buntkowsky

Vogel

2020

Molecules

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This review gives an overview of current trends in the investigation of small guest molecules, confined in neat and functionalized mesoporous silica materials by a combination of solid-state NMR and relaxometry with other physico-chemical techniques. The reported guest molecules are water, small alcohols, and carbonic acids, small aromatic and heteroaromatic molecules, ionic liquids, and surfactants. They are taken as characteristic role-models, which are representatives for the typical classes of organic molecules. It is shown that this combination delivers unique insights into the structure, arrangement, dynamics, guest-host interactions, and the binding sites in these confined systems, and is probably the most powerful analytical technique to probe these systems.

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Section: Porous Host Materialsmentioning

confidence: 99%

Section: Simple Liquids In Confinementmentioning

confidence: 99%

Section: Figurementioning

confidence: 99%

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Small Molecules, Non-Covalent Interactions, and Confinement

Buntkowsky

Vogel

2020

Molecules

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“…Post grafting requires an additional synthesis step, and in many cases cannot reach the grafting density of the co‐condensation strategy. Furthermore, post grafting suffers from the restricted accessibility of the inner pore surface, due to mass transport limitation of the reactants in the pores and pore blockings . In contrary, co‐condensation approaches offer the possibility of high grafting densities.…”

Section: Introductionmentioning

confidence: 99%

“…Generally, homo‐condensation between the linker molecules is preferred over condensation of the linker molecules resulting to an incorporation onto the surface silica. Wrong timings and ratios during synthesis can lead to disordered and unstable pore systems …”

Section: Introductionmentioning

confidence: 99%

Biofunctionalization of Nano Channels by Direct In‐Pore Solid‐Phase Peptide Synthesis

Brodrecht

Breitzke

Gutmann

et al. 2018

Chemistry A European J

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Diatom biosilica are highly complex inorganic/organic hybrid materials. To get deeper insights on their structure at a molecular level, model systems that mimic the complex natural compounds were synthesized and characterized. A simple and efficient peptide immobilization strategy was developed, which uses a well-ordered porous silica material as a support and commercially available Fmoc-amino acids, similar to the known solid-phase peptide synthesis. As an example, Fmoc-glycine and Fmoc-phenylalanine are immobilized on the silica support. The success of functionalization was investigated by C CP MAS and Si CP MAS solid-state NMR. Thermogravimetric analysis (TGA) and elemental analysis (EA) were performed to quantify the functionalization. Changes of the specific surface area, pore volume, and pore diameters in all modification steps were studied by Brunauer-Emmett-Teller based nitrogen adsorption-desorption measurements (BET). The combination of the analytical methods provided high grafting densities of 2.1±0.2 molecules/nm on the surface. Furthermore, they allowed for monitoring chemical changes on the pore surface and changes of the pore properties of the material during the different functionalization steps. This universal approach is suitable for the selective synthesis of pores with tunable surface-peptide functionalization, with applications to the synthesis of a big variety of silica-peptide model systems, which in the future may lead to a deeper understanding of complex biological systems.

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Structural Insights into Peptides Bound to the Surface of Silica Nanopores

Brodrecht

Kumari

Thankamony

et al. 2019

Chemistry A European J

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The structure and surface functionalization of biologically relevant silica‐based hybrid materials was investigated by 2D solid‐state NMR techniques combined with dynamic nuclear polarization (DNP). This approach was applied to a model system of mesoporous silica, which was modified through in‐pore grafting of small peptides by solid‐phase peptide synthesis (SPPS). To prove the covalent binding of the peptides on the surface, DNP‐enhanced solid‐state NMR was used for the detection of 15N NMR signals in natural abundance. DNP‐enhanced heterocorrelation experiments with frequency switched Lee–Goldburg homonuclear proton decoupling (1H–13C and 1H–15N CP MAS FSLG HETCOR) were performed to verify the primary structure and configuration of the synthesized peptides. 1H FSLG spectra and 1H‐29Si FSLG HETCOR correlation spectra were recorded to investigate the orientation of the amino acid residues with respect to the silica surface. The combination of these NMR techniques provides detailed insights into the structure of amino acid functionalized hybrid compounds and allows for the understanding for each synthesis step during the in‐pore SPPS.

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Chemically Modified Silica Materials as Model Systems for the Characterization of Water-Surface Interactions

Cited by 18 publications

References 81 publications

Small Molecules, Non-Covalent Interactions, and Confinement

Small Molecules, Non-Covalent Interactions, and Confinement

Biofunctionalization of Nano Channels by Direct In‐Pore Solid‐Phase Peptide Synthesis

Structural Insights into Peptides Bound to the Surface of Silica Nanopores

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