Towards in-situ detection of catalytic turnover from a single, isolated nanoparticle in the transmission electron microscope

Research output: Book/ReportPh.D. thesis

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Abstract

The industrialised world relies heavily on heterogeneous catalysis as the backbone technology facilitating the production of everything from fuels and chemicals to polymers and synthetic fertilisers. It is, therefore, only natural that significant resources are being spent on understanding how to improve the efficiency of these processes as well as develop new processes that could help address problems such as the environmental crisis.
Much scientific effort has been put into investigation of the relationship between structure and activity of the small metal nanoparticles on which catalysis happens industrially, but existing research methods lack the ability to study isolated nanoparticles due to the issue of scaling down and detecting products from one single nanoparticle. The atomic insight cavity array reactor (ATOMICAR) attempts to address this shortcoming of scientific methods by delivering a platform for the study of isolated nanoparticles in the transmission electron microscope where high-resolution imaging can be combined with spectroscopic techniques. This should allow for unprecedented investigations of catalysis at the single-nanoparticle level that could help elucidate the structure-function relationship, and hopefully, provide new insights for the development of catalysts.
This thesis is the result of the work with the ATOMICAR device towards the realisation of single nanoparticle catalysis and has been divided into two general topics.
The first topic is the benchmarking of the reactor that subsequently led to the study of gas leakage at the interface between graphene and silicon dioxide. This interface is important in several emerging technologies as well as for the use of the ATOMICAR device as it constitutes the gas-barrier between the reactor and the vacuum of the electron microscope.
The second topic describes the work towards the realisation of single nanoparticle catalysis including topics like isolation of nanoparticles and cavity sealing with 2D materials. This work has been many-faceted and progress has been made in several areas, resulting in a fairly long workflow. The chapter also gives a report on the latest measurement where catalysis was finally observed in the ATOMICAR device, and ends with a reflection on the current status of the project.
Original languageEnglish
PublisherDepartment of Physics, Technical University of Denmark
Number of pages130
Publication statusPublished - 2023

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