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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

Stephen T. Skowron

Thomas W. Chamberlain

Johannes Biskupek

Ute Kaiser



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