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Open AccessArticle

Tetrathiafulvalene: A Gate to the Mechanochemical Mechanisms of Electron Transfer Reactions

Department of Chemistry & Biochemistry, Old Dominion University, 4402 Elkhorn Avenue, Norfolk, VA 23529, USA
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Crystals 2020, 10(6), 482; https://doi.org/10.3390/cryst10060482
Received: 20 May 2020 / Revised: 1 June 2020 / Accepted: 2 June 2020 / Published: 5 June 2020
(This article belongs to the Special Issue Charge Transfer Crystals)
This report describes aspects of our previous studies of the mechanochemical synthesis of charge transfer complexes of the electron donor tetrathiafulvalene, which are relevant to the use of laboratory X-ray powder diffraction for ex situ monitoring of mechanochemical reactions toward investigating their mechanisms. In particular, the reaction of tetrathiafulvalene and chloranil was studied under neat mechanochemical conditions and liquid-assisted grinding with diethyl ether (1 μL/mg). The product in both cases is the green tetrathiafulvalene chloranil polymorph and the mechanism of the redox reaction is presumably the same. However, while the kinetic profile of the neat mechanochemical synthesis was fitted with a second-order rate law, that of the overall faster liquid-assisted grinding reaction was fitted with the Ginstling-Brounshtein 3D diffusion-controlled model. Hence, the diffusional processes and mass transfer bringing the reactants together and separating them from products must be different. Diffraction measurements sensitive to crystalline phases and amorphous material, combined with in situ monitoring by spectroscopic techniques, will ultimately afford a better understanding of mechanochemical reaction mechanisms, a hot topic in mechanochemistry. View Full-Text
Keywords: tetrathiafulvalene; charge transfer complexes; electron-transfer reactions; mechanochemistry; reaction mechanisms; solid-state reaction models tetrathiafulvalene; charge transfer complexes; electron-transfer reactions; mechanochemistry; reaction mechanisms; solid-state reaction models
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Chen, R.; Gokus, M.K.; Pagola, S. Tetrathiafulvalene: A Gate to the Mechanochemical Mechanisms of Electron Transfer Reactions. Crystals 2020, 10, 482.

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