Abstract

Beyond lithium-ion battery (LIB) chemistries demand new electrode materials exhibiting unique features to accommodate the larger and/or multivalent active ions. Zeolite-templated carbon (ZTC) is an ordered microporous carbon scaffold that is molecularly thin, electrically conductive, and covalently connected in three dimensions. Its narrow pore size distribution is centered at 1.2 nm, permitting the introduction and ultrafast conduction of large molecular guests. In this work, we demonstrate the serviceability of ZTC as a stable cathode material across wide voltage ranges for both bulky, polyatomic anions (as in dual-ion batteries, DIBs, and/or hybrid capacitors, HCs) and multivalent cations (e.g., magnesium-ion batteries, MIBs) in high energy density and high power density electrochemical cells. Charge storage proceeds by a purely capacitive mechanism at the surface of ZTC, mated with the faradaic mechanism of metal plating and stripping at the anode. A suite of techniques including solid-state NMR spectroscopy sheds insight into the role of the solvent, anion, and cation in electrochemical insertion/deinsertion of the active ions within the microporous framework of ZTC. Figure 1

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