Along with the widening application and growing market size of energy storage devices, the development of costeffective rechargeable batteries with a high level of operational safety has become a major challenge. To this end, an all-solid-state battery (ASSB), which is composed of a thin film instead of a liquid, is an attractive candidate. In this study, we investigated a facile method for preparing sodium superionic conductor structured Na 1+x Zr 2 Si x P 3−x O 12 (0 ≤ x ≤ 3, NZSP). Various attempts were made to improve the sinterability of NZSP, but the results are still unsatisfactory. We employed the reaction sintering method so that the phase formation and densification proceeded simultaneously, resulting in the densification of NZSP with minimal impurities. Furthermore, we successfully substituted rare-earth elements (REs) into the Zr site of the NZSP to tune its structural properties in the nanoscale and improve its ionic conductivity. Electrochemical impedance spectroscopy results confirmed the improvement of the ionic conductivity of both the pristine NZSP and the RE-doped variant, indicating the effectiveness of reaction sintering. When reaction sintering and RE substitution were employed together, La-doped NZSP was an attractive solid electrolyte for application in ASSBs. Our results highlight the effectiveness of reaction sintering for obtaining an impurity-free and highly dense multicomponent compound.
Anode‐free lithium metal batteries (AFLMBs) show promise as a means of further enhancing the energy density of current lithium‐ion batteries, as they do not require conventional graphite anodes. The anode‐free configuration, however, suffers from inferior chemical stability of the solid electrolyte interphase (SEI) layer and experiences inhomogeneous lithium deposition during charge/discharge processes, resulting in rapid capacity fading. To address these issues, a carbonized polydopamine (CPD) coating is applied to the copper current collector. The CPD‐coated copper current collector promotes highly efficient and reversible lithium plating and stripping processes, resulting in a densely packed lithium deposition that significantly improves cycling stability. The anode‐free full cell, consisting of CPD‐coated copper current collector and a LiFePO4 cathode, demonstrates significantly improved electrochemical performance, with a capacity retention of more than 63% after 100 cycles at a current rate of 0.3C. The stability of the SEI layer and the presence of lithiophilic sites are verified through a range of techniques, including optical microscopy, Raman spectroscopy, X‐ray photoelectron spectroscopy, chronoamperometry, and electrochemical impedance spectroscopy. Based on these collective findings, it can be inferred that the use of CPD coating provides a simple way to enhance the electrochemical performance of AFLMBs.
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