Stephen T. Skowron
Chemical Reactions of Molecules Promoted and Simultaneously Imaged by the Electron Beam in Transmission Electron Microscopy
Skowron, Stephen T.; Chamberlain, Thomas W.; Biskupek, Johannes; Kaiser, Ute; Besley, Elena; Khlobystov, Andrei N.
Authors
Thomas W. Chamberlain
Johannes Biskupek
Ute Kaiser
Professor ELENA BESLEY ELENA.BESLEY@NOTTINGHAM.AC.UK
Professor of Theoretical Computational Chemistry
ANDREI KHLOBYSTOV ANDREI.KHLOBYSTOV@NOTTINGHAM.AC.UK
Professor of Chemical Nanoscience
Abstract
The main objective of this Account is to assess the challenges of transmission electron microscopy (TEM) of molecules, based on over 15 years of our work in this field, and to outline the opportunities in studying chemical reactions under the electron beam (e-beam). During TEM imaging of an individual molecule adsorbed on an atomically thin substrate, such as graphene or a carbon nanotube, the e-beam transfers kinetic energy to atoms of the molecule, displacing them from equilibrium positions. Impact of the e-beam triggers bond dissociation and various chemical reactions which can be imaged concurrently with their activation by the e-beam and can be presented as stop-frame movies. This experimental approach, which we term ChemTEM, harnesses energy transferred from the e-beam to the molecule via direct interactions with the atomic nuclei, enabling accurate predictions of bond dissociation events and control of the type and rate of chemical reactions. Elemental composition and structure of the reactant molecules as well as the operating conditions of TEM (particularly the energy of the e-beam) determine the product formed in ChemTEM processes, while the e-beam dose rate controls the reaction rate. Because the e-beam of TEM acts simultaneously as a source of energy for the reaction and as an imaging tool monitoring the same reaction, ChemTEM reveals atomic-level chemical information, such as pathways of reactions imaged for individual molecules, step-by-step and in real time; structures of illusive reaction intermediates; and direct comparison of catalytic activity of different transition metals filmed with atomic resolution. Chemical transformations in ChemTEM often lead to previously unforeseen products, demonstrating the potential of this method to become not only an analytical tool for studying reactions, but also a powerful instrument for discovery of materials that can be synthesized on preparative scale.
Citation
Skowron, S. T., Chamberlain, T. W., Biskupek, J., Kaiser, U., Besley, E., & Khlobystov, A. N. (2017). Chemical Reactions of Molecules Promoted and Simultaneously Imaged by the Electron Beam in Transmission Electron Microscopy. Accounts of Chemical Research, 50(8), 1797-1807. https://doi.org/10.1021/acs.accounts.7b00078
Journal Article Type | Article |
---|---|
Acceptance Date | Jul 11, 2017 |
Online Publication Date | Jul 11, 2017 |
Publication Date | Aug 15, 2017 |
Deposit Date | Sep 17, 2019 |
Journal | Accounts of Chemical Research |
Print ISSN | 0001-4842 |
Electronic ISSN | 1520-4898 |
Publisher | American Chemical Society |
Peer Reviewed | Peer Reviewed |
Volume | 50 |
Issue | 8 |
Pages | 1797-1807 |
DOI | https://doi.org/10.1021/acs.accounts.7b00078 |
Keywords | General Chemistry; General Medicine |
Public URL | https://nottingham-repository.worktribe.com/output/2468405 |
Publisher URL | https://pubs.acs.org/doi/10.1021/acs.accounts.7b00078 |
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