The shuttling of soluble lithium polysulfides between the electrodes leads to serious capacity fading and excess use of electrolyte, which severely bottlenecks practical use of Li-S batteries. Here, selective catalysis is proposed as a fundamental remedy for the consecutive solid-liquid-solid sulfur redox reactions. The proof-of-concept Indium (In)-based catalyst targetedly decelerates the solid-liquid conversion, dissolution of elemental sulfur to polysulfides, while accelerates the liquid-solid conversion, deposition of polysulfides into insoluble Li2 S, which basically reduces accumulation of polysulfides in electrolyte, finally inhibiting the shuttle effect. The selective catalysis is revealed, experimentally and theoretically, by changes of activation energies and kinetic currents, modified reaction pathway together with the probed dynamically changing catalyst (LiInS2 catalyst), and gradual deactivation of the In-based catalyst. The In-based battery works steadily over 1000 cycles at 4.0 C and yields an initial areal capacity up to 9.4 mAh cm-2 with a sulfur loading of ≈9.0 mg cm-2 .

/pdf/selective-catalysis-remedies-polysulfide-shuttling-in-51pdwc75ce.pdf

Selective Catalysis Remedies Polysulfide Shuttling in Lithium-Sulfur Batteries.

Efficient electrode materials, that combine high power and high energy, are the crucial requisites of sodium‐ion batteries (SIBs), which have unwrapped new possibilities in the areas of grid‐scale energy storage. Hard carbons (HCs) are considered as the leading candidate anode materials for SIBs, however, the primary challenge of slow charge‐transfer kinetics at the low potential region (<0.1 V) remains unresolved till date, and the underlying structure–performance correlation is under debate. Herein, ultrafast sodium storage in the whole‐voltage‐region (0.01–2 V), with the Na+ diffusion coefficient enhanced by 2 orders of magnitude (≈10–7 cm2 s–1) through rationally deploying the physical parameters of HCs using a ZnO‐assisted bulk etching strategy is reported. It is unveiled that the Na+ adsorption energy (Ea) and diffusion barrier (Eb) are in a positive and negative linear relationship with the carbon p‐band center, respectively, and balance of Ea and Eb is critical in enhancing the charge‐storage kinetics. The charge‐storage mechanism in HCs is evidenced through comprehensive in(ex) situ techniques. The as prepared HCs microspheres deliver a record high rate performance of 107 mAh g–1 @ 50 A g–1 and unprecedented electrochemical performance at extremely low temperature (426 mAh g–1 @ −40 °C).

Enabling Fast Na+ Transfer Kinetics in the Whole‐Voltage‐Region of Hard‐Carbon Anodes for Ultrahigh‐Rate Sodium Storage

Thermally Stable and Nonflammable Electrolytes for Lithium Metal Batteries: Progress and Perspectives

Hard carbons, as one of the most commercializable anode materials for sodium‐ion batteries (SIBs), have to deal with the trade‐off between the rate capability and specific capacity or initial Columbic efficiency (ICE), and the fast performance decline at low temperature (LT) remains poorly understood. Here, a comprehensive regulation on the interfacial/bulk electrochemistry of hard carbons through atomic Zn doping is reported, which demonstrates a record‐high reversible capacity (546 mAh g−1), decent ICE (84%), remarkable rate capability (140 mAh g−1 @ 50 A g−1), and excellent LT capacity (443 mAh g−1 @ −40 °C), outperforming the state‐of‐the‐art literature. This work reveals that the Zn doping can generally induce a local electric field to enable fast bulk Na+ transportation, and meanwhile catalyze the decomposition of NaPF6 to form a robust inorganic‐rich solid‐electrolyte interphase, which elaborates the underlying origin of the boosted electrochemical performance. Importantly, distinguished from room temperature, the intrinsic Na+ migration/desolvation ability of the electrolyte is disclosed to be the crucial rate‐determining factors for the SIB performance at LT. This work provides a fundamental understanding on the charge‐storage kinetics at varied temperatures.

Zinc Single‐Atom‐Regulated Hard Carbons for High‐Rate and Low‐Temperature Sodium‐Ion Batteries

Metallic Na (K) are considered a promising anode materials for Na‐metal and K‐metal batteries because of their high theoretical capacity, low electrode potential, and abundant resources. However, the uncontrolled growth of Na (K) dendrites severely damages the stability of the electrode/electrolyte interface, resulting in battery failure. Herein, a heterogeneous interface layer consisting of metal vanadium nanoparticles and sodium sulfide (potassium sulfide) is introduced on the surface of a Na (K) foil (i.e., Na2S/V/Na or K2S/V/K). Experimental studies and theoretical calculations indicate that a heterogeneous Na2S/V (K2S/V) protective layer can effectively improve Na (K)‐ion adsorption and diffusion kinetics, inhibiting the growth of Na (K) dendrites during Na (K) plating/stripping. Based on the novel design of the heterogeneous layer, the symmetric Na2S/V/Na cell displays a long lifespan of over 1000 h in a carbonate‐based electrolyte, and the K2S/V/K electrode can operate for over 1300 h at 0.5 mA cm–2 with a capacity of 0.5 mAh cm–2. Moreover, the Na full cell (Na3V2(PO4)3||Na2S/V/Na) exhibits a high energy density of 375 Wh kg–1 and a high power density of 23.5 kW kg–1. The achievements support the development of heterogeneous protective layers for other high‐energy‐density metal batteries.

Artificial Heterogeneous Interphase Layer with Boosted Ion Affinity and Diffusion for Na/K‐Metal Batteries

https://onlinelibrary.wiley.com/doi/pdf/10.1002/smsc.202000063

What Is the Right Carbon for Practical Anode in Alkali Metal Ion Batteries

Carbonaceous Electrode Materials

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What Is the Right Carbon for Practical Anode in Alkali Metal Ion Batteries

Carbonaceous Electrode Materials