Pressureless all-solid-state Na/S batteries with self-supporting Na_(5)YSi_(4)O_(12) scaffolds

The development of reliable and affordable all-solid-state sodium metal batteries(ASS-SMBs)requires suitable solid-state electrolytes with cost-efficient processing and stabilized electrode/electrolyte interfaces.Here,an integrated porous/dense/porous Na_(5)YSi_(4)O_(12)(NYS)trilayered scaffold is designed and fabricated by tape casting using aqueous slurries.In this template-based NYS scaffold,the dense layer in the middle serves as a separator and the porous layers on both sides accommodate the active materials with their volume changes during the charge/discharge processes,increasing the contact area and thus enhancing the utilization rate and homogenizing the current distribution.The Na/NYS/Na symmetric cells with the Pb-coated NYS scaffold exhibit significantly reduced interfacial impedance and superior critical current density of up to 3.0 mA cm^(-2)against Na metal owing to enhanced wettability.Furthermore,the assembled Na/NYS/S full cells operated without external pressure at room temperature showed a high initial discharge capacity of 970 mAh g^(-1)and good cycling stability with a capacity of 600 mAh g^(-1)after 150 cycles(based on the mass of sulfur).This approach paves the way for the realization of economical and practical ASS-SMBs from the perspective of ceramic manufacturing.

Enhanced room-temperature Na^(+) ionic conductivity in Na_(4.92)Y_(0.92)Zr_(0.08)Si_(4)O_(12)

Developing cost-effective and reliable solid-state sodium batteries with superior performance is crucial for stationary energy storage.A key component in facilitating their application is a solid-state electrolyte with high conductivity and stability.Herein,we employed aliovalent cation substitution to enhance ionic conductivity while preserving the crystal structure.Optimized substitution of Y^(3+)with Zr^(4+)in Na_(5)YSi_(4)O_(12) introduced Naþion vacancies,resulting in high bulk and total conductivities of up to 6.5 and 3.3 mS cm^(-1),respectively,at room temperature with the composition Na_(4.92)Y_(0.92)Zr_(0.08)Si_(4)O_(12)(NYZS).NYZS shows exceptional electrochemical stability(up to 10 V vs.Naþ/Na),favorable interfacial compatibility with Na,and an excellent critical current density of 2.4 mA cm^(-2).The enhanced conductivity of Naþions in NYZS was elucidated using solid-state nuclear magnetic resonance techniques and theoretical simulations,revealing two migration routes facilitated by the synergistic effect of increased Naþion vacancies and improved chemical environment due to Zr^(4+)substitution.NYZS extends the list of suitable solid-state electrolytes and enables the facile synthesis of stable,low-cost Naþion silicate electrolytes.