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Safe and high-energy-density all solid-state lithium metal batteries (ASSLMBs) are great in demand for future electrical vehicle and grid energy storage. The compatibility of electrode-electrolyte interface is a critical factor influencing the electrochemical performance of ASSLMBs. Herein, we propose a plastic super-conductive carrier to deter untoward reaction between Li anode and Li1.5Al0.5Ge1.5(PO4)3 (LAGP) electrolyte by in-situ solidifying succinonitrile-based plastic interlayer with Li6.4La3Zr2Al0.24O12 (LLZAO) nanowires (l-SN). The method of in-situ solidification promises the low interfacial resistance. The l-SN interlayer can not only act as a physical obstacle to isolate LAGP pellet from Li metal, but also provide three-dimensional ion channels to regulate the transfer of Li ions, delivering an uniform Li ion distribution for dendrite-free Li deposition. The Li|l-SN|LAGP|l-SN|Li symmetric cell can stably cycle for 240 h without short circuit at room temperature (R.T). This approach enables a high specific capacity of 152.5 mAh g−1 at 0.1C for Li|l-SN|LAGP|l-SN|LiFePO4 cells at R.T. Furthermore, the integrated ASSLMBs show excellent cyclic stability at 40 °C with an initial discharge capacity of 168.4 mAh g−1 at 0.5C and retention of 93.17% after 100 cycles. The super-ionic property at the interface makes excellent rate performance of ASSLMBs at 40 °C. This strategy is facile and efficient in promising safe and outstanding ASSLMBs and also has some referential values for other unstable electrolyte interface beyond LAGP.

Bulk graphitic carbon materials with expanded interlayer spacing and abundant defects may serve as efficient anodes with high areal capacities for sodium-ion batteries (SIBs). However, obtaining long-range order in bulk graphitic carbon materials with expanded interlayer spacing is extremely difficult. Herein, an explosive decomposition method is demonstrated to realize thermally reduced graphene oxide (rGO) paper with tuned interlayer spacing. The in-situ temperature-dependent X-ray diffraction (td-XRD) was utilized to establish the correlation between heating rate and interlayer spacing. Based on td-XRD results, free-standing graphene paper (FSG) was synthesized at 450°C under a high heating rate of 70°C/min. The FSG exhibits a highly porous structure made of graphene flakes with abundant surface epoxy groups with an overall interlayer spacing of 0.38–0.39 nm. The rGO flakes in FSG are separated by large voids that provide fast mass transport pathways and allow expansion/contraction of crystallites upon reversible Na intercalation. The FSG was utilized directly as anodes without any binder and conductive agent and delivered an excellent reversible capacity of 290 mAh/g at a current density of 50 mA/g. Moreover, the FSG exhibited excellent foldability and rollability to create high areal density anodes, delivering an areal capacity of 0.62 mAh/cm2 at a current density of 100 μA/cm2. These results open the door to fabricate graphene material-based carbon anodes with tunable interlayer spacing for high-performance SIBs.

With the growing demand for high-energy-density lithium-ion batteries, layered lithium-rich cathode materials with high specific capacity and low cost have been widely regarded as one of the most attractive candidates for next-generation lithium-ion batteries. However, issues such as voltage decay, capacity loss and sluggish reaction kinetics have hindered their further commercialization for decades. Intensive investigations have been devoted to developing high-performance lithium-rich cathode materials, highlighting the importance of improvement strategies as a potential approach. Herein, we summarize various strategies for improving performances of layered lithium-rich cathode materials for next-generation high-energy-density lithium-ion batteries. These include surface engineering, elemental doping, composition optimization, structure engineering and electrolyte additives, with emphasis on the effect and functional mechanism of corresponding techniques. In the subsequent section, we illustrate opportunities and challenges for designing high-performance lithium-rich cathode materials and bridging the gap between the laboratory and practical applications.

© 2020 Elsevier B.V. Sodium iron hexacyanoferrate (NaFeHCF) has been considered as a potential cathode for sodium-ion batteries owing to its low-cost and easily prepared procedure. However, it is still challenging to achieve long cyclic stability and superior rate capability, and the sodium storage mechanism of sodium-rich NaFeHCF is still elusive. Herein, a sodium-rich NaFeHCF with rhombohedral structure is presented with excellent electrochemical performances within 2.0–4.2 ​V. The specific capacity of ~115 ​mA ​h ​g−1 is obtained by utilizing two plateaus around 2.9 and 4.06 ​V, respectively. Remarkable rate performance from 10 to 4000 ​mA ​g−1 and 1000 cycles with high capacity retention is achieved as well. Synchrotron powder X-ray diffraction (PXRD) and structural refinement reveals that sodium-ions occupy three different sites (interstitial, face and edge) in rhombohedral unit cell, which contribute different capacities on different plateaus during Na+ extractions. Moreover, the rhombohedral structure is well-maintained after long-term Na+ extractions/insertions and reversible phase transitions with small volume variation are observed through in-situ synchrotron PXRD. The kinetic properties of Na+ in rhombohedral unit cell are identified by ab-initio molecular dynamics method and density functional theory calculations, which indicate that Na+ transport on three-dimensional diffusion paths, thus enabling the outstanding rate performance of NaFeHCF.