Combining Nanoplasmonics and Nanofluidics for Single Particle Catalysis
Licentiatavhandling, 2018

Nanoparticles are, due to their large exposed surface area, widely used in the field of heterogeneous catalysis where they accelerate and steer chemical reactions. Although catalysis has been known about for centuries, the scrutiny of catalysts under realistic application conditions is still a major challenge. This difficulty originates from the fact that real catalyst materials are very complex, often consisting of large ensembles of nanoparticles that all are unique. Furthermore, the typically used macroscopic reactors in catalysis studies gives rise to locally, at the level of the active site, ill-defined reactant concentrations and diffusion limitations.

To overcome these limitations, on one hand, techniques are being developed that are sensitive enough to probe individual catalytic particles and that at the same time can operate under realistic reaction conditions. On the other hand, strategies to more carefully control the amount and structure of catalyst material, as well as to precisely control mass transport to and from the active catalyst, are being investigated by scaling down the size of the used chemical reactor. To further push the limit of downsizing, in this thesis, I present a miniaturized reactor platform based on nanofluidic channels that have been carefully decorated with catalytic nanoparticles, and that is integrated with plasmonic nanospectroscopy readout. This optical technique relies on the nanoscale phenomenon known as the Localized Surface Plasmon Resonance (LSPR) and enables the study of individual metal nanoparticles in operando by means of dark-field scattering spectroscopy.

As the first step in this development, we constructed a nanofluidic device with integrated plasmonic nanoparticles to detect minute changes in the liquid flowing through the channels, as well as molecules binding to the nanoparticles. As the second step, we developed the nanofluidic system with an integrated heater and to facilitate gas flow through the nanochannels with the possibility to connect to a mass spectrometer for on-line product analysis. This system was then successfully used to correlate activity with surface and bulk oxidation state changes taking place on individual catalytic Cu and Pt nanoparticles during CO oxidation, measured by means of plasmonic nanospectroscopy. To this end, in a separate study, I also employed the plasmonic approach to study the oxidation process of Cu nanoparticles both experimentally and by electrodynamics simulations.

heterogeneous catalysis

plasmonic sensing

nanoreactor

CO oxidation

dark field scattering spectroscopy

nanocatalyst

LSPR

nanofluidics

Cu oxidation

single particle catalysis

PJ-salen, Fysik Origo, Chalmers Tekniska Högskola, Göteborg
Opponent: Per-Anders Carlsson, Institutionen för Kemi och kemiteknik, Chalmers Tekniska Högskola, Göteborg

Författare

David Albinsson

Chalmers, Fysik, Kemisk fysik

Single Particle Nanoplasmonic Sensing in Individual Nanofluidic Channels

Nano Letters,; Vol. 16(2016)p. 7857-7864

Artikel i vetenskaplig tidskrift

David Albinsson, Sara Nilsson, Tomasz J. Antosiewicz, and Christoph Langhammer, Plasmonic Heterodimers for Drift-Free Sensing of Cu Nanoparticle Oxidation and the Nanoscale Kirkendall Effect

David Albinsson, Stephan Bartling, Sara Nilsson, Henrik Ström, Joachim Fritzsche, Christoph Langhammer, Nanofluidic Reactors for Single Particle Catalysis

Single Particle Catalysis in Nanoreactors (SPCN)

Knut och Alice Wallenbergs Stiftelse, 2016-01-01 -- 2020-12-31.

Single Nanoparticle Catalysis, SINCAT

Europeiska kommissionen (Horisont 2020), 2016-01-01 -- 2020-12-31.

Styrkeområden

Nanovetenskap och nanoteknik

Ämneskategorier

Fysik

Nanoteknik

Kemi

Infrastruktur

Chalmers materialanalyslaboratorium

Nanotekniklaboratoriet

Utgivare

Chalmers tekniska högskola

PJ-salen, Fysik Origo, Chalmers Tekniska Högskola, Göteborg

Opponent: Per-Anders Carlsson, Institutionen för Kemi och kemiteknik, Chalmers Tekniska Högskola, Göteborg

Mer information

Senast uppdaterat

2018-11-15