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Achieving Fast kinetics and enhanced Li storage capacity for Ti3C2O2 by intercalation of quinone molecules Edirisuriya M. D. Siriwardane, Ilker Demiroglu, Cem Sevik, and Deniz Cakir ACS Appl. Energy Mater., Just Accepted Manuscript • DOI: 10.1021/acsaem.8b01801 • Publication Date (Web): 04 Jan 2019 Downloaded from http://pubs.acs.org on January 14, 2019
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ACS Applied Energy Materials
Achieving Fast kinetics and enhanced Li storage capacity for Ti3C2O2 by intercalation of quinone molecules Edirisuriya M. D. Siriwardane,† Ilker Demiroglu,‡ Cem Sevik,‡ and Deniz Çakır∗,† †Department of Physics and Astrophysics, University of North Dakota, Grand Forks, North Dakota 58202, USA ‡Department of Mechanical Engineering, Faculty of Engineering, Anadolu University, Eskisehir, TR 26555, Turkey E-mail: *
[email protected] Abstract Using first-principles calculations, we demonstrated that high lithium storage capacity and fast kinetics are achieved for Ti3 C2 O2 by preintercalating organic molecules. As a proof-of-concept, two different quinone molecules, namely 1,4-Benzoquinone (C6 H4 O2 ) and Tetrafluoro-1,4-benzoquinone (C6 F4 O2 ) were selected as the molecular linkers to demonstrate the feasibility of this interlayer engineering strategy for energy storage. As compared to Ti3 C2 O2 bilayer without linker molecules, our pillared structures facilitate a much faster ion transport, promising a higher charge/discharge rate for Li. For example, while the diffusion barrier of a single Li ion within pristine Ti3 C2 O2 bilayer is at least 1.0 eV, it becomes 0.3 eV in pillared structures, which is comparable and even lower than that of commercial materials. At high Li concentrations, the calculated diffusion barriers are as low as 0.4 eV. Out-of-plane migration of Li ions is hindered
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due to large barrier energy with a value of around 1-1.35 eV. Concerning storage capacity, we can only intercalate one monolayer of Li within pristine Ti3 C2 O2 bilayer. In contrast, pillared structures offer significantly higher storage capacity. Our calculations showed that at least two layers of Li can be intercalated between Ti3 C2 O2 layers without forming bulk Li and losing the pillared structure upon Li loading/unloading. A small change in the in-plane lattice parameters (
