Homologous Heterointerfaces and Interfacial Chemical Bonding for Greatly Improved Initial Coulombic Efficiency in Sodium Storage

作者：Liang Cao, Mingjing Chu, Xin Xu, Wenqing Zhao, Yue Dai, Xianglai Cui, Qingyu Li, Huilong Dong, Hongbo Geng · 发表于：ACS Sustainable Chemistry & Engineering · 年份：2025 · DOI：10.1021/acssuschemeng.5c02903 · 被引用次数：3 · 研究领域：Advancements in Battery Materials、Chemical Synthesis and Characterization、Nuclear materials and radiation effects

Transition metal chalcogenide (TMC), an appealing anode alternative for high-energy-density sodium-ion batteries (SIBs), still encounters considerable challenges in practical applications, such as poor reaction reversibility, sluggish Na + transport, the notorious shuttle effect, and inferior structural stability. Herein, we propose an ambidextrous approach of internal homologous heterointerface (Ni 3 S 2 /Ni 9 S 8 ) engineering and exterior interfacial chemical bonding (Ni–S–C) modulation to settle the above bottlenecks. In this configuration, a built-in electric field inside the homologous heterostructure enhances charge transport, reduces the Na diffusion barrier, and facilitates mass transfer. Meanwhile, the interfacial chemical bonding between NiS x and the outer graphene scaffold effectively stabilizes the soluble NaPS and improves the durability of the structure, resulting in high reaction reversibility and a desirable cycle lifespan. Consequently, the prepared electrode exhibits a remarkable ICE value (94%) with a high specific capacity (366.9 mAh g –1 at 10 A g –1 after 1200 cycles). Additionally, the working mechanism is comprehensively revealed by combining in situ analysis and theoretical calculations. This study provides a light way to prepare elaborate TMC materials for advanced SIBs.