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Counting molecules in nano test tubes: a method for determining the activation parameters of thermally driven reactions through direct imaging

DOI: 10.1039/D1CC03827C DOI Help

Authors: Kayleigh L. Y. Fung (University of Nottingham) , Stephen T. Skowron (University of Nottingham) , Christopher S. Allen (Diamond Light Source; University of Oxford) , Andrei N. Khlobystov (University of Nottingham)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemical Communications , VOL 38

State: Published (Approved)
Published: September 2021
Diamond Proposal Number(s): 22887 , 23260 , 25251

Abstract: A methodology for measuring activation parameters of a thermally driven chemical reaction by direct imaging and counting reactant molecules has been developed. The method combines the use of single walled carbon nanotubes (SWNTs) as a nano test tube, transmission electron microscopy (TEM) as an imaging tool, and a heating protocol that decouples the effect of the electron beam from the thermal activation. Polycyclic aromatic perchlorocoronene molecules are stable within SWNTs at room temperature, allowing imaging of individual molecules before and after each heating cycle between 500–600 °C. Polymerisation reaction rates can be determined at different temperatures simply by counting the number of molecules, resulting in an enthalpy of activation of 104 kJ mol−1 and very large entropic contributions to the Gibbs free energy of activation. This experimental methodology provides a link between reactions at the single-molecule level and macroscopic chemical kinetics parameters, through filming the chemical reaction in direct space.

Subject Areas: Chemistry, Technique Development

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E02-JEM ARM 300CF

Added On: 28/09/2021 09:50

Discipline Tags:

Physical Chemistry Technique Development - Chemistry Chemistry

Technical Tags:

Microscopy Electron Microscopy (EM) Transmission Electron Microscopy (TEM)