Chemistry of Materials · 2017 · 252 citations · 64 references
Natural SciencesMaterials EngineeringMaterials ScienceElectrochemical EngineeringElectrochemistryMaterials ChemistryAnode MaterialsBattery MaterialsElectrochemical Energy StorageElectrode MaterialsEnergy StorageEnergy Storage MaterialsAnode Material SelectionEnergy DensityGraphite AnodesHigh-capacity Anode MaterialsMechanical ProcessingNuclear Magnetic Resonance Studies
The quest for low-cost and large-scale stationary storage of electricity has led to a surge of reports on novel batteries comprising exclusively highly abundant chemical elements. Aluminum-based systems, <i>inter</i> alia, are appealing because of the safety and affordability of aluminum anodes. In this work, we examined the recently proposed aluminum-ionic liquid-graphite architecture. Using <sup>27</sup>Al nuclear magnetic resonance, we confirmed that AlCl<sub>4</sub><sup>-</sup> acts as an intercalating species. Although previous studies have focused on graphitic cathodes, we analyzed the practicality of achievable energy densities and found that the AlCl<sub>3</sub><sup>-</sup>based ionic liquid is a capacity-limiting anode material. By focusing on both the graphitic cathode and the AlCl<sub>3</sub><sup>-</sup>based anode, we improved the overall energy density. First, high cathodic capacities of ≤150 mAh g<SUP>-1</SUP> and energy efficiencies of 90% at high electrode loadings of at least 10 mg cm<SUP>-2</SUP> were obtained with natural, highly crystalline graphite flakes, which were subjected to minimal mechanical processing. Second, the AlCl<sub>3</sub> content in the ionic liquid was increased to its maximal value, which essentially doubled the energy density of the battery, resulting in a cell-level energy density of ≤62 Wh kg<SUP>-1</SUP>. The resulting batteries were also characterized by high power densities of at least 489 W kg<SUP>-1</SUP>.
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