A commentary on an anode-free cell design with electrochemically stable sodium borohydride solid electrolyte and pelletized aluminium current collector for sodium all-solid-state batteries is presented. First, the viable strategies for implementing anode-free configuration utilizing solid-state electrolytes are briefly reviewed. Then, the remarkable work of Meng et al. on designing an anode-free sodium all-solid-state battery is elucidated. Finally, the significance of Meng’s work is discussed.
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Commentary
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Open Access
Research Article
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As the persistent concerns regarding sluggish reaction kinetics and insufficient conductivities of sulfur cathodes in all-solid-state Li–S batteries (ASSLSBs), numerous carbon additives and solid-state electrolytes (SSEs) have been incorporated into the cathode to facilitate ion/electron pathways around sulfur. However, this has resulted in a reduced capacity and decomposition of SSEs. Therefore, it is worth exploring neotype sulfur hosts with electronic/ionic conductivity in the cathode. Herein, we present a hybrid cathode composed of few-layered S/MoS2/C nanosheets (<5 layers) that exhibits high-loading and long-life performance without the need of additional carbon additives in advanced ASSLSBs. The multifunctional MoS2/C host exposes the abundant surface for intimate contacting sites, in situ-formed LixMoS2 during discharging as mixed ion/electron conductive network improves the S/Li2S conversion, and contributes extra capacity for the part of active materials. With a high active material content (S + MoS2/C) of 60 wt% in the S/MoS2/C/Li6PS5Cl cathode composite (the carbon content is only ~3.97 wt%), the S/MoS2/C electrode delivers excellent electrochemical performance, with a high reversible discharge capacity of 980.3 mAh g−1 (588.2 mAh g−1 based on the whole cathode weight) after 100 cycles at 100 mA g−1. The stable cycling performance is observed over 3500 cycles with a Coulombic efficiency of 98.5% at 600 mA g−1, while a high areal capacity of 10.4 mAh cm−2 is achieved with active material loading of 12.8 mg cm−2.
The point-to-point contact mechanism in all-solid-state Li-S batteries (ASSLSBs) is not as efficient as a liquid electrolyte which has superior mobility in the electrode, resulting in a slower reaction kinetics and inadequate ionic/electronic conduction network between the S (or Li2S), conductive carbon, and solid-state electrolytes (SSEs) for achieving a swift (dis)charge reaction. Herein, a series of hybrid ionic/electronic conduction triple-phase interfaces with transition metal and nitrogen co-doping were designed. The graphitic ordered mesoporous carbon frameworks (TM-N-OMCs; TM = Fe, Co, Ni, and Cu) serve as hosts for Li2S and Li6PS5Cl (LPSC) and provide abundant reaction sites on the triple interface. Results from both experimental and computational research display that the combination of Cu-N co-dopants can promote the Li-ion diffusion for rapid transformation of Li2S with adequate ionic (6.73 × 10−4 S·cm−1)/electronic conductivities (1.77 × 10−2 S·cm−1) at 25 °C. The as-acquired Li2S/Cu-N-OMC/LPSC electrode exhibits a high reversible capacity (1147.7 mAh·g−1) at 0.1 C, excellent capacity retention (99.5%) after 500 cycles at 0.5 C, and high areal capacity (7.08 mAh·cm−2).
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