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Nanofluidic Scattering Microscopy an...

Altenburger, Bjorn,

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Nanofluidic Scattering Microscopy and Spectroscopy for Single Particle Catalysis /

Record Type:	Electronic resources : Monograph/item
Title/Author:	Nanofluidic Scattering Microscopy and Spectroscopy for Single Particle Catalysis // Bjorn Altenburger.
Author:	Altenburger, Bjorn,
Description:	1 electronic resource (97 pages)
Notes:	Source: Dissertations Abstracts International, Volume: 86-04, Section: B.
Contained By:	Dissertations Abstracts International86-04B.
Subject:	Metals. -
Online resource:	https://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=31599326
ISBN:	9798342126847

Nanofluidic Scattering Microscopy and Spectroscopy for Single Particle Catalysis /
Altenburger, Bjorn,

Nanofluidic Scattering Microscopy and Spectroscopy for Single Particle Catalysis /Bjorn Altenburger. - 1 electronic resource (97 pages)

Source: Dissertations Abstracts International, Volume: 86-04, Section: B.

Nanoparticles are a fundamental asset in modern society, and a cornerstone in global industries where they contribute significantly to the path towards sustainable energy and products. Their ability to facilitate and steer chemical reactions is studied in the field of heterogeneous catalysis, where these tiny particles are characterized regarding their activity and selectivity. However, the characterization is often conducted on large ensembles of particles, thereby disregarding their structural heterogeneity, which possibly leads to erroneous structure-function correlations. Since it is one goal of catalysis research to find "superparticles" with exceptional performance, the need for dedicated single particle studies where the influence of, e.g., shape, size and surface structure is investigated in detail, is obvious.Methods like fluorescence microscopy, X-ray diffraction/scattering, electron microscopy and plasmonic sensing are commonly used for single particle investigations in catalysis. These methods detect electrons or photons that carry information either on the reactant molecules, the product molecules, changes to the catalyst particle itself or the particle surrounding. However, none of these methods provides direct single particle activity information without either using plasmonic enhancement effects that may also impact the studied reaction itself and limit the range of catalyst materials that can be studied, or using fluorescence that limits reaction conditions to ultralow concentrations and to a narrow range of reactions.The overarching goal of the work presented in this thesis has been to develop an optical microscopy technique that can quantitatively measure catalytic activity, and in the longer term even selectivity, of a single nanoparticle, without the limitations of existing single particle techniques. At the core of this method - Nanofluidic Scattering Microscopy - are nanofluidic channels that can accurately control the transport of molecules to and from a single, catalytically active, particle localized inside a channel. As a second key trait, the unique light scattering properties of nanochannels render them highly sensitive to refractive index changes of the fluid inside them. Hence, when a catalytic reaction alters the molecular composition of the fluid in a nanochannel, its light scattering characteristics change and reveal in this way the catalytic performance of the nanoparticle, which here is demonstrated for H2O2 decomposition over on single Pt particles. Furthermore, resolving the scattered light spectrally, as I do in Nanofluidic Scattering Spectroscopy, spectral fingerprints of a catalytic reaction can be resolved, as demonstrated for the catalytic reduction of fluorescein on a single Au nanoparticle.In the wake of these developments, I also have developed a new fluidic platform, chip holder and microscopy setup to harness the full potential of micro- and nanofluidics in combination with optical microscopy and spectroscopy applied to single particle catalysis investigations.

English

ISBN: 9798342126847Subjects--Topical Terms:

601053
Metals.

Nanofluidic Scattering Microscopy and Spectroscopy for Single Particle Catalysis /
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520 $a Nanoparticles are a fundamental asset in modern society, and a cornerstone in global industries where they contribute significantly to the path towards sustainable energy and products. Their ability to facilitate and steer chemical reactions is studied in the field of heterogeneous catalysis, where these tiny particles are characterized regarding their activity and selectivity. However, the characterization is often conducted on large ensembles of particles, thereby disregarding their structural heterogeneity, which possibly leads to erroneous structure-function correlations. Since it is one goal of catalysis research to find "superparticles" with exceptional performance, the need for dedicated single particle studies where the influence of, e.g., shape, size and surface structure is investigated in detail, is obvious.Methods like fluorescence microscopy, X-ray diffraction/scattering, electron microscopy and plasmonic sensing are commonly used for single particle investigations in catalysis. These methods detect electrons or photons that carry information either on the reactant molecules, the product molecules, changes to the catalyst particle itself or the particle surrounding. However, none of these methods provides direct single particle activity information without either using plasmonic enhancement effects that may also impact the studied reaction itself and limit the range of catalyst materials that can be studied, or using fluorescence that limits reaction conditions to ultralow concentrations and to a narrow range of reactions.The overarching goal of the work presented in this thesis has been to develop an optical microscopy technique that can quantitatively measure catalytic activity, and in the longer term even selectivity, of a single nanoparticle, without the limitations of existing single particle techniques. At the core of this method - Nanofluidic Scattering Microscopy - are nanofluidic channels that can accurately control the transport of molecules to and from a single, catalytically active, particle localized inside a channel. As a second key trait, the unique light scattering properties of nanochannels render them highly sensitive to refractive index changes of the fluid inside them. Hence, when a catalytic reaction alters the molecular composition of the fluid in a nanochannel, its light scattering characteristics change and reveal in this way the catalytic performance of the nanoparticle, which here is demonstrated for H2O2 decomposition over on single Pt particles. Furthermore, resolving the scattered light spectrally, as I do in Nanofluidic Scattering Spectroscopy, spectral fingerprints of a catalytic reaction can be resolved, as demonstrated for the catalytic reduction of fluorescein on a single Au nanoparticle.In the wake of these developments, I also have developed a new fluidic platform, chip holder and microscopy setup to harness the full potential of micro- and nanofluidics in combination with optical microscopy and spectroscopy applied to single particle catalysis investigations.
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