Abstract

The development of high-performance anode materials for lithium-ion batteries is a critical aspect of advancing energy storage technology. This study presents a novel approach to improve the charge capacity of anodes by harnessing the reversible growth of the solid electrolyte interface (SEI). This work focuses on cobalt sulfide (Co9S8) nanoparticles incorporated into a porous carbon nanotube (CNT) structure. Through a two-step pyrolysis process, Co9S8CNT composites, characterized by their conductive and mechanically robust CNT matrix are successfully synthesized. These Co9S8CNT anodes exhibit excellent initial charge capacity (560.5 mAh g−1 at 100 mA g−1) and remarkable stability, with a charge capacity of 633 mAh g−1 after 1000 cycles at 1000 mA g−1, accompanied by a Coulombic efficiency exceeding 99 %. Notably, this investigation reveals that the growth of the SEI plays a pivotal role in enhancing the charge capacity. Through in-situ Raman spectroscopy and other analytical techniques, it is suggested that the reversible reduction of organic solvent molecules within the large polymeric SEI is responsible for the increased charge capacity. This unique phenomenon is characterized by changes in the SEI's composition, driven by the charge and discharge processes. This study is a novel attempt to report a SEI's reversible growth that results in improved charge capacity, contrasting with prior research where SEI growth typically leads to capacity loss. Understanding this stable system provides valuable insights into increasing the cycle life and charge capacity of anodes, not only for transition metal sulfides but also for broader applications in energy storage.

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