Tuning Single‐Molecule Dynamics in Functionalized Mesoporous Silica

Lebold, Timo; Mühlstein, Lea; Blechinger, Julia; Riederer, Melanie; Amenitsch, Heinz; Köhn, Ralf; Peneva, Kalina; Müllen, Kläus; Michaelis, Jens; Bräuchle, Christoph; Bein, Thomas

doi:10.1002/chem.200801380

Cited by 31 publications

(39 citation statements)

References 52 publications

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“…[416] for a review). In these experiments, luminescent probe molecules were incorporated in as‐synthesized mesoporous silica, and their diffusion along the channels was followed with a fluorescence microscope . The passage of dye molecules between channels was detected, thus proving that the pores were connected .…”

Section: Empty Space Architecturesmentioning

confidence: 99%

Supramolecular Organization in Confined Nanospaces

Tabacchi

2018

ChemPhysChem

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Empty spaces are abhorred by nature, which immediately rushes in to fill the void. Humans have learnt pretty well how to make ordered empty nanocontainers, and to get useful products out of them. When such an order is imparted to molecules, new properties may appear, often yielding advanced applications. This review illustrates how the organized void space inherently present in various materials: zeolites, clathrates, mesoporous silica/organosilica, and metal organic frameworks (MOF), for example, can be exploited to create confined, organized, and self-assembled supramolecular structures of low dimensionality. Features of the confining matrices relevant to organization are presented with special focus on molecular-level aspects. Selected examples of confined supramolecular assemblies - from small molecules to quantum dots or luminescent species - are aimed to show the complexity and potential of this approach. Natural confinement (minerals) and hyperconfinement (high pressure) provide further opportunities to understand and master the atomistic-level interactions governing supramolecular organization under nanospace restrictions.

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Section: Empty Space Architecturesmentioning

confidence: 99%

Supramolecular Organization in Confined Nanospaces

Tabacchi

2018

ChemPhysChem

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“…Angewandte Chemie more, Lebold et al observed that the mobility of TDI molecules can increase or decrease depending on the functional groups attached to the mesoporous silica wall. [59] The authors explained their findings in terms of shielding of the hydroxy groups of the silica surface in combination with changes in the rigidity of the micellar packing in the silica film and directional interactions between the functional groups and the TDI molecules. In summary, single-molecule detection of dye molecules in porous structures reveals a wealth of information about the topology, nanoscale connectivity, and accessibility of the channels of a porous catalyst material.…”

Section: Spatial Heterogeneities In Catalysismentioning

confidence: 99%

Chemical Imaging of Spatial Heterogeneities in Catalytic Solids at Different Length and Time Scales

2009

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Knowledge of spatiotemporal gradients in heterogeneous catalysts is of paramount importance for the rational design of new and more sustainable catalytic processes. Heterogeneities resulting in space- and time-dependent phenomena occur at different length scales; that is, at the level of catalytic reactors (mm to m), catalyst bodies (microm to mm), catalyst grains (nm to microm), and active sites and metal (oxide) particles (A to nm). This Review documents the recent advances in the development of space- and time-resolved spectroscopic methods for imaging spatial heterogeneities within catalytic processes at these four length scales. Particular emphasis will be on the use of magnetic resonance, optical, and synchrotron-based methods, their capabilities in providing spatial resolution (1D and 2D imaging) and depth profiling (3D imaging) as well as on their time-resolved application, potential for single-molecule and nanoparticle detection, and use under reaction conditions. The Review ends with future prospects on spectroscopic markers for catalytic activity, label-free spectroscopy, tomography at the nanoscale, and correlative microscopic approaches.

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“…Single molecule microscopy provides an excellent means to study the effects the functionalization excerts on incorporated guest molecules. 66 Different approaches can be used to influence the mobility of the guest molecule. First, the influence of the functionalization density on the diffusion dynamics of the dye can be examined.…”

Section: Analyzing the Translational Orientational And Spectral Diffmentioning

confidence: 99%

“…66 Fig. 6c shows the diffusion data for aliphatic functional groups with different alkyl chain lengths (methyl, ethyl and propyl).…”

Section: Analyzing the Translational Orientational And Spectral Diffmentioning

confidence: 99%

The complexity of mesoporous silica nanomaterials unravelled by single molecule microscopy

Lebold

Michaelis

Bräuchle

2011

Phys. Chem. Chem. Phys.

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Mesoporous silica nanomaterials are a novel class of materials that offer a highly complex porous network with nanometre-sized channels into which a wide amount of differently sized guests can be incorporated. This makes them an ideal host for various applications for example in catalysis, chromatography and nanomedicine. For these applications, analyzing the host properties and understanding the complicated host-guest interactions is of pivotal importance. In this perspective we review some of our recent work that demonstrates that single molecule microscopy techniques can be utilized to characterize the porous silica host with unprecedented detail. Furthermore, the single molecule studies reveal sample heterogeneities and are a highly efficient tool to gain direct mechanistic insights into the host-guest interactions. Single molecule microscopy thus contributes to a thorough understanding of these nanomaterials enabling the development of novel tailor-made materials and hence optimizing their applicability significantly.

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Tuning Single‐Molecule Dynamics in Functionalized Mesoporous Silica

Cited by 31 publications

References 52 publications

Supramolecular Organization in Confined Nanospaces

Supramolecular Organization in Confined Nanospaces

Chemical Imaging of Spatial Heterogeneities in Catalytic Solids at Different Length and Time Scales

The complexity of mesoporous silica nanomaterials unravelled by single molecule microscopy

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