Collaborative Hollow Porous Structure Design and N Doping to Achieve a Win–Win Situation of “Stable” and “Fast” Lithium Battery

Abstract

Polymer-derived SiOC materials are widely regarded as a new generation of anodes owing to their high specific capacity, low discharge platform, tunable chemical/structural composition, and good structural stability. However, tailoring the structure of SiOC to improve its electrochemical performance while simultaneously achieving elemental doping remains a challenge. Besides, the lithium storage mechanism and the structural evolution process of SiOC are still not fully understood due to its complex structure. In this study, a hollow porous SiOCN (Hp-SiOCN) featuring abundant oxygen defects is successfully prepared, achieving both the creation of a hollow porous structure and nitrogen element doping in one step, finally enhancing the structural stability and improving the lithium storage kinetics of Hp-SiOCN. In addition, the formation of a fully reversible structural unit, SiO₃C—N, through the chemical interaction between N and Si/C, showcases a strong lithium adsorption capacity. Taking advantage of these combined benefits, the as-prepared Hp-SiOCN electrode delivers a reversible specific capacity of 412 mAh g^–1 (93% capacity retention) after 500 cycles at 1.0 A g^–1 and exhibited only 4% electrode expansion. This work offers valuable mechanistic insights into the synergistic optimization of elemental doping and structural design in SiOC, paving the way for advanced developments in battery technology.

Keywords

doping / hollow porous structure / lithium batteries / reaction kinetics / SiOC

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2024 The Author(s). SusMat published by Sichuan University and John Wiley & Sons Australia, Ltd.