Regulating Electron Filling and Orbital Occupancy of Anti-Bonding States of Transition Metal Nitride Heterojunction for High Areal Capacity Lithium-Sulfur Full Batteries.

The commercialization of lithium-sulfur (Li-S) battery is seriously hindered by the shuttle behavior of lithium (Li) polysulfide, slow conversion kinetics, and Li dendrite growth. Herein, a novel hierarchical p-type iron nitride and n-type vanadium nitride (p-Fe2N/n-VN) heterostructure with optimal electronic structure, confined in vesicle-like N-doped nanofibers (p-Fe2N/n-VN⊂PNCF), is meticulously constructed to work as "one stone two birds" dual-functional hosts for both the sulfur cathode and Li anode. As demonstrated, the d-band center of high-spin Fe atom captures more electrons from V atom to realize more π* and moderate σ* bond electron filling and orbital occupation; thus, allowing moderate adsorption intensity for polysulfides and more effective d-p orbital hybridization to improve reaction kinetics. Meanwhile, this unique structure can dynamically balance the deposition and transport of Li on the anode; thereby, more effectively inhibiting Li dendrite growth and promoting the formation of a uniform solid electrolyte interface. The as-assembled Li-S full batteries exhibit the conspicuous capacities and ultralong cycling lifespan over 2000 cycles at 5.0 C. Even at a higher S loading (20 mg cm-2) and lean electrolyte (2.5 µL mg-1), the full cells can still achieve an ultrahigh areal capacity of 16.1 mAh cm-2 after 500 cycles at 0.1 C.

Solid-State Electrolytes: Probing Interface Regulation from Multiple Perspectives.

Solid-state electrolytes (SSEs), as the heart of all-solid-state batteries (ASSBs), are recognized as the next-generation energy storage solution, offering high safety, extended cycle life, and superior energy density. SSEs play a pivotal role in ion transport and electron separation. Nonetheless, interface compatibility and stability issues pose significant obstacles to further enhancing ASSB performance. Extensive research has demonstrated that interface control methods can effectively elevate ASSB performance. This review delves into the advancements and recent progress of SSEs in interfacial engineering over the past years. We discuss the detailed effects of various regulation strategies and directions on performance, encompassing enhancing Li+ mobility, reducing energy barriers, immobilizing anions, introducing interlayers, and constructing unique structures. This review offers fresh perspectives on the development of high-performance lithium-metal ASSBs.

A restricted dynamic surface self-reconstruction toward high-performance of direct seawater oxidation.

The development of highly efficient electrocatalysts for direct seawater splitting with bifunctionality for inhibiting anodic oxidation reconstruction and selective oxygen evolution reactions is a major challenge. Herein, we report a direct seawater oxidation electrocatalyst that achieves long-term stability for more than 1000 h at 600 mA/cm2@η600 and high selectivity (Faraday efficiency of 100%). This catalyst revolves an amorphous molybdenum oxide layer constructed on the beaded-like cobalt oxide interface by atomic layer deposition technology. As demonstrated, a new restricted dynamic surface self-reconstruction mechanism is induced by the formation a stable reconstructed Co-Mo double hydroxide phase interface layer. The device assembled into a two-electrode flow cell for direct overall seawater electrolysis maintained at 1 A/cm2@1.93 V for 500 h with Faraday efficiency higher than 95%. Hydrogen generation rate reaches 419.4 mL/cm2/h, and the power consumption (4.62 KWh/m3 H2) is lower than that of pure water (5.0 KWh/m3 H2) at industrial current density.