Ribbon-Ordered Superlattice Enables Reversible Anion Redox and Stable High-Voltage Na-Ion Battery Cathodes.

High-voltage layered oxide cathodes attract great attention for sodium-ion batteries (SIBs) due to the potential high energy density, but high voltage usually leads to rapid capacity decay. Herein, a stable high-voltage NaLiNiMnTiO cathode with a ribbon-ordered superlattice is reported, and the intrinsic coupling mechanism between structure evolution and the anion redox reaction (ARR) is revealed. Li introduction constructs a special Li-O-Na configuration activating reversible nonbonded O 2p (|O)-type ARR and regulates the structure evolution way, enabling the reversible Li ions out-of-layer migration instead of the irreversible transition metal ions out-of-layer migration.

A Unique Wide-Spacing Fence-Type Superstructure for Robust High-Voltage O3-Type Sodium Layered Cathode.

Enhancing the energy density of layered oxide cathode materials is of great significance for realizing high-performance sodium-ion batteries and promoting their commercial application. Lattice oxygen redox at high voltage usually enables a high capacity and energy density. But the structural degradation, severe voltage decay, and the resultant poor cycling performance caused by irreversible oxygen release seriously restrict the practical application.

Reversing Zincophobic/Hydrophilic Nature of Metal-N-C via Metal-Coordination Interaction for Dendrite-Free Zn Anode with High Depth-of-Discharge.

Dendrite-free Zn metal anodes with high depth-of-discharge (DoD) and robust cycle performances are highly desired for the practical application of aqueous Zn-ion batteries. Herein, the zincophobic/hydrophilic nature of Metal-N-C through manipulating the electronic interactions between metal and coordination atoms is successfully reversed, thereby fabricating a zincophilic/hydrophobic asymmetric Zn-N-C (consisting of a Zn center coordinated with 3 pyridinic N atoms and 1 pyrrolic N atom) host, which realizes uniformed Zn deposition and a long lifespan with high DoD. The experimental and theoretical investigations demonstrate weakened interaction between pyrrolic N and metal center in the asymmetric Zn-N-C triggers downshift of the Zn 3d-band-center and a new localization nonbonding state in the N and C 2p-band, resulting in preferred Zn adsorption to water adsorption.

Electron Redistribution Enables Redox-Resistible Li PS Cl towards High-Performance All-Solid-State Lithium Batteries.

Sulfide electrolytes with high ionic conductivity hold great promise for all-solid-state lithium batteries. However, the parasitic redox reactions between sulfide electrolyte and Li metal result in interfacial instability and rapid decline of the battery performance. Herein, a redox-resistible Li PS Cl (LPSC) electrolyte is created by regulating the electron distribution in LPSC with Mg and F incorporation.