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ACS Applied Materials & Interfaces Page 6 of 17 Zeolite-Templated Carbon as the Cathode for a High Energy Density Dual-Ion Battery Romain J.‐C. Dubey†‡, Jasmin Nüssli†‡, Laura Piveteau†‡, Kostiantyn V. Kravchyk†‡, Marta D. Ros‐ sell∥, Marco Campanini∥, Rolf Erni∥, Maksym V. Kovalenko†‡* and Nicholas P. Stadie#* †Laboratory of Inorganic Chemistry, Department of Chemistry and Applied Biosciences, ETH Zürich, CH‐8093 Zürich, Switzerland ‡Laboratory for Thin Films and Photovoltaics, Empa, Swiss Federal Laboratories for Materials Science & Technology, CH‐8600 Dübendorf, Switzerland ∥Electron Microscopy Center, Empa, Swiss Federal Laboratories for Materials Science & Technology, CH‐8600 Düben‐ dorf, Switzerland #Department of Chemistry & Biochemistry, Montana State University, Bozeman, Montana, 59717, United States ABSTRACT: Dual‐ion batteries (DIBs) are electrochemical energy storage devices that operate by the simultaneous partici‐ pation of two different ion species at the anode and the cathode and rely on the use of an electrolyte that can withstand the high operation potential of the cathode. Under such conditions at the cathode, issues associated with irreversible capacity loss and the formation of solid‐electrolyte interphase (SEI) at the surface of highly porous electrode materials are far less significant than at lower potentials, permitting the exploration of high surface area, permanently porous framework materials as effective charge storage media. This concept is investigated herein by employing zeolite‐templated carbon (ZTC) as the cathode in a dual‐ion battery based on a potassium bis(fluorosulfonyl)imide (KFSI) electrolyte. Anion (FSI‐) insertion within the pore network during electrochemical cycling is confirmed by NMR spectroscopy, and the maximum charge capacity is found to be proportional to surface area and micropore volume by comparison to other microporous carbon materials. Full‐ cells based on ZTC as the cathode exhibit both high specific energy (up to 176 Wh kg‐1, 79.8 Wh L‐1) and high specific power (up to 3945 W kg‐1, 1095 W L‐1), stable cycling performance over hundreds of cycles, and reversibility within the potential range of 2.65‐4.7 V vs. K/K+. KEYWORDS: potassium, bis(fluorosulfonyl)imide, capacitive, microporous, electrode, electrochemical energy storage INTRODUCTION Dual‐ion batteries1‐5 (DIBs) are an emerging class of electro‐ chemical energy storage devices that are distinguished from common “shuttle‐type” or “rocking chair” batteries such as lithium‐ion batteries (LIBs) that rely on the participation of only a single type of ion (e.g., Li+) at both electrodes. In a DIB cell, two types of ions (a cation and anion pair) co‐mingle in the bulk electrolyte in the discharged state. Upon charging, the large (typically polyatomic) anions are oxidatively in‐ serted into the cathode material, a process that occurs at high potential relative to the reversible electroplating, alloying, or insertion reaction of the cation at the anode. The mainstay of research into compounds that can readily host anionic species has remained focused on nonporous solids such as graphite6‐ 15, nanostructured graphitic materials16‐20, amorphous carbon materials (e.g., hard carbon21, mesocarbon microbeads22, and microbead films23), hydrocarbons (e.g., polycyclic aromatic hydrocarbons24, 25 and aromatic diamines26), conductive poly‐ mers27‐29, and some metals (e.g., metal fluorides30). A 3D po‐ rous carbon has been investigated as a high stability current collector for graphite‐based DIBs.31 On the contrary, little at‐ tention has been paid to the use of high surface area mi‐ croporous32 materials as exclusively capacitive‐type cathode materials in DIBs (although redox‐active metal‐organic frameworks (MOFs) have indeed begun to be explored33‐35). In this work, we draw attention to two key features of DIBs that lend great potential promise to conductive microporous materials carrying a large accessible inner surface to serve as a high‐capacity and high‐rate capability, purely capacitive cathode material: (i) the high working potential of the ca‐ thodic reaction occurring at the porous material surface and (ii) the large size of the anions typically employed. The high potential of anion insertion/de‐insertion significantly miti‐ gates the irreversible loss of energy density associated with excessive solid‐electrolyte interphase (SEI) formation during the first several cycles, a well‐known problem associated with the low potential adsorption of cations at the surface of po‐ rous anode materials in shuttle‐type batteries.36‐39 Further‐ more, the oxidative insertion of anions is, in general, a notori‐ ously challenging reaction to perform reversibly and/or at high rates within condensed solid‐state media (as compared to the reductive insertion of smaller cations). This observa‐ tion is often attributed mainly to the larger size of the anions employed,40 although such size effects have been shown to be complexly related to other electrolyte effects, such as ion‐pair formation and self‐aggregation.41 These observations to‐ gether strongly incentivize the exploration of highly porous ACS Paragon Plus EnvironmentPDF Image | Zeolite-Templated Carbon as the Cathode
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