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Item Hydrogen-Type Binding Sites in Carbonaceous Electrodes for Rapid Lithium Insertion(American Chemical Society, 2023-08) McGlamery, Devin; McDaniel, Charles; Xu, Wei; Stadie, Nicholas P.Direct pyrolysis of coronene at 800 °C produces low-surface-area, nanocrystalline graphitic carbon containing a uniquely high content of a class of lithium binding sites referred to herein as “hydrogen-type” sites. Correspondingly, this material exhibits a distinct redox couple under electrochemical lithiation that is characterized as intermediate-strength, capacitive lithium binding, centered at ∼0.5 V vs Li/Li+. Lithiation of hydrogen-type sites is reversible and electrochemically distinct from capacitive lithium adsorption and from intercalation-type binding between graphitic layers. Hydrogen-type site lithiation can be fully retained even up to ultrafast current rates (e.g., 15 A g–1, ∼40 C) where intercalation is severely hampered by ion desolvation kinetics; at the same time, the bulk nature of these sites does not require a large surface area, and only minimal electrolyte decomposition occurs during the first charge/discharge cycle, making coronene-derived carbon an exceptional candidate for high-energy-density battery applications.Item Biochar as a Renewable Substitute for Carbon Black in Lithium-Ion Battery Electrodes(American Chemical Society, 2022-09) Kane, Seth; Storer, Aksiin; Xu, Wei; Ryan, Cecily; Stadie, Nicholas P.Lignin-derived biochar was prepared and characterized toward potential applications as a conductive electrode additive and active lithium host material within lithium-ion batteries (LIBs). This biochar was specifically selected for its high electrical conductivity, which is comparable to that of common conductive carbon black standards (e.g., Super P). Owing to its high electrical conductivity, this biochar serves as an effective conductive additive within electrodes comprising graphite as the active material, demonstrating slightly improved cell efficiency and rate capability over those of electrodes using carbon black as the additive. Despite its effectiveness as a conductive additive in LIB anodes, preliminary results show that the biochar developed in this work is not suitable as a direct replacement for carbon black as a conductive additive in LiFePO4 cathodes. This latter insufficiency may be due to differences in particle geometry between biochar and carbon black; further optimization is necessary to permit the application of biochar as a general-purpose conductive additive in LIBs. Nevertheless, these investigations combined with an assessment of greenhouse gas emissions from biochar production show that replacing carbon black with biochar can be an effective method to improve the sustainability of LIBs.Item Biochar as a Renewable Substitute for Carbon Black in Lithium-Ion Battery Electrodes(American Chemical Society, 2022-09) Kane, Seth; Storer, Aksiin; Xu, Wei; Ryan, Cecily; Stadie, Nicholas P.Lignin-derived biochar was prepared and characterized towards potential applications as a conductive electrode additive and active lithium host material within lithium-ion batteries (LIBs). This biochar was specifically selected for its high electrical conductivity, which is comparable to that of common conductive carbon black standards (e.g., Super P). Owing to its high electrical conductivity, this biochar serves as an effective conductive additive within electrodes comprised of graphite as the active material, demonstrating slightly improved cell efficiency and rate capability over electrodes using carbon black as the additive. Despite its effectiveness as a conductive additive in LIB anodes, preliminary results show that the biochar developed in this work is not suitable as a direct replacement for carbon black as a conductive additive in LiFePO4 (LFP) cathodes. This latter insufficiency may be due to differences in particle 2 geometry between biochar and carbon black; further optimization is necessary to permit the application of biochar as a general-purpose conductive additive in LIBs. Nevertheless, these investigations combined with an assessment of greenhouse gas emissions from biochar production show that replacing carbon black with biochar can be an effective method to improve the sustainability of LIBs.