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Rechargeable garnet-based solid-state Li batteries hold immense promise as non-flammable, non-toxic, and high-energy-density energy storage systems, employing Li7La3Zr2O12 (LLZO) with a garnet-type structure as the solid-state electrolyte. Despite substantial progress in this field, the advancement and eventual commercialization of garnet-based solid-state Li batteries is impeded by void formation at the LLZO/Li interface at practical current densities and areal capacities beyond 1 mA cm−2 and 1 mAh cm−2, resulting in limited cycling stability and the emergence of Li dendrites. Additionally, developing a fabrication approach for thin LLZO electrolytes to achieve high energy density remains paramount. To address these critical challenges, herein, we present a facile methodology for fabricating self-standing, 50-µm thick, porous LLZO membranes with a small pore size of ca. 2.3 µm and an average porosity of 51%, resulting in a specific surface area of 1.3 µm−1, the highest reported to date. The use of such LLZO membranes significantly increases the Li/LLZO contact area, effectively mitigating void formation. This methodology combines two key elements: (i) the use of small pore formers of ca. 1.5 µm, and (ii) the use of ultrafast sintering, which circumvents ceramics overdensification using rapid heating/cooling rates of ca. 50 °C per second. The fabricated porous LLZO membranes demonstrate exceptional cycling stability in a symmetrical Li/LLZO/Li cell configuration, exceeding 600 hours of continuous operation at a current density of 0.1 mA cm−2. 

Dual-ion hybrid capacitors (DIHCs) are a promising class of electrochemical energy storage devices intermediate between batteries and supercapacitors, exhibiting both high energy and power density, and generalizable across wide chemistries beyond lithium. In this study, a model carbon framework material with a periodic structure containing exclusively 1.2 nm width pores, zeolite-templated carbon (ZTC), was investigated as the positive electrode for the storage of a range of anions relevant to DIHC chemistries. Screening experiments were carried out across 21 electrolyte compositions within a common stable potential window of 3.0–4.0 V vs. Li/Li+ to determine trends in capacity as a function of anion and solvent properties. To achieve fast rate capability, a binary solvent balancing a high dielectric constant with a low viscosity and small molecular size was used; optimized full-cells based on LiPF6 in binary electrolyte exhibited 146 Wh kg−1 and >4000 W kg−1 energy and power densities, respectively.