Synergistically Coupling Atomic‐Level Defect‐Manipulation and Nanoscopic‐Level Interfacial Engineering Enables Fast and Durable Sodium Storage

Abstract

AbstractThrough inducing interlayer anionic ligands and functionally modifying conductive carbon‐skeleton on the transition metal chalcogenides (TMCs) parent to achieve atomic‐level defect‐manipulation and nanoscopic‐level architecture design is of great significance, which can broaden interlayer distance, optimize electronic structure, and mitigate structural deformation to endow high‐efficiency battery performance of TMCs. Herein, an intriguing 3D biconcave hollow‐tyre‐like anode constituted by carbon‐packaged defective‐rich SnSSe nanosheet grafting onto Aspergillus niger spores‐derived hollow‐carbon (ANDC@SnSSe@C) is reported. Systematically experimental investigations and theoretical analyses forcefully demonstrate the existence of anion Se ligand and outer‐carbon all‐around encapsulation on the ANDC@SnSSe@C can effectively yield abundant structural defects and Na+‐reactivity sites, accelerate rapid ion migration, widen interlayer spacing, as well as relieve volume expansion, thus further resolving the critical issues throughout the charge–discharge processes. As anticipated, as‐fabricated ANDC@SnSSe@C anode contributes extraordinary reversible capacity, wonderful cyclic lifespan with 83.4% capacity retention over 2000 cycles at 20.0 A g−1, and exceptional rate capability. A series of correlated kinetic investigations and ex situ characterizations deeply reveal the underlying springheads for the ion‐transport kinetics, as well as synthetically elucidate phase‐transformation mechanism of the ANDC@SnSSe@C. Furthermore, the ANDC@SnSSe@C‐based sodium ion full cell and hybrid capacitor offer high‐capacity contribution and remarkable energy‐density output, indicative of its great practicability.