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Editors' Choice-Mechanistic Elucidation of Anion Intercalation into Graphite from Binary-Mixed Highly Concentrated Electrolytes via Complementary F-19 MAS NMR and XRD Studies

Haneke, Lukas; Frerichs, Joop Enno; Heckmann, Andreas; Lerner, Michael M.; Akbay, Taner; Ishihara, Tatsumi; Hansen, Michael Ryan; Winter, Martin; Placke, Tobias


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<oai_dc:dc xmlns:dc="http://purl.org/dc/elements/1.1/" xmlns:oai_dc="http://www.openarchives.org/OAI/2.0/oai_dc/" xmlns:xsi="http://www.w3.org/2001/XMLSchema-instance" xsi:schemaLocation="http://www.openarchives.org/OAI/2.0/oai_dc/ http://www.openarchives.org/OAI/2.0/oai_dc.xsd">
  <dc:creator>Haneke, Lukas</dc:creator>
  <dc:creator>Frerichs, Joop Enno</dc:creator>
  <dc:creator>Heckmann, Andreas</dc:creator>
  <dc:creator>Lerner, Michael M.</dc:creator>
  <dc:creator>Akbay, Taner</dc:creator>
  <dc:creator>Ishihara, Tatsumi</dc:creator>
  <dc:creator>Hansen, Michael Ryan</dc:creator>
  <dc:creator>Winter, Martin</dc:creator>
  <dc:creator>Placke, Tobias</dc:creator>
  <dc:date>2020-01-01</dc:date>
  <dc:description>Dual-graphite batteries have emerged as promising candidate for sustainable energy storage due to their potentially low costs and absence of toxic materials. However, the mechanism of anion intercalation and the structures of the resulting graphite intercalation compounds (GICs) are still not well understood. Here, we systematically evaluate the anion intercalation characteristics into graphite for three highly concentrated electrolytes containing LiPF6, LiTFSI and their equimolar binary mixture. The binary mixture exhibits a significantly enhanced capacity retention and improved intercalation kinetics compared to the single-salt electrolytes in graphite divide divide Li metal cells. In situ X-ray diffraction studies prove the formation of stage 1-GICs and a homogeneous distribution of anions within graphite. From ex situ solid-state F-19 magic-angle spinning (MAS) nuclear magnetic resonance (NMR) measurements, GICs can be identified at various states-of-charge (SOCs). The F-19 chemical shifts of intercalated anions indicate no significant charge transfer between anion and graphite. The observed narrow F-19 linewidths of the GIC-signals are most likely caused by a high translational and/or rotational mobility of the intercalates. Furthermore, the F-19 MAS NMR studies allow the identification of the molar ratios for PF6- and TFSI- anions intercalated into graphite, suggesting a preferred intercalation of PF6- anions, especially at lower SOCs. (C) 2020 The Author(s). Published on behalf of The Electrochemical Society by IOP Publishing Limited. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited.</dc:description>
  <dc:identifier>https://aperta.ulakbim.gov.trrecord/4785</dc:identifier>
  <dc:identifier>oai:zenodo.org:4785</dc:identifier>
  <dc:rights>info:eu-repo/semantics/openAccess</dc:rights>
  <dc:rights>http://www.opendefinition.org/licenses/cc-by</dc:rights>
  <dc:source>JOURNAL OF THE ELECTROCHEMICAL SOCIETY 167(14)</dc:source>
  <dc:title>Editors' Choice-Mechanistic Elucidation of Anion Intercalation into Graphite from Binary-Mixed Highly Concentrated Electrolytes via Complementary F-19 MAS NMR and XRD Studies</dc:title>
  <dc:type>info:eu-repo/semantics/article</dc:type>
  <dc:type>publication-article</dc:type>
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