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ALD Derived Li2O Layer Stabilizing Solid Electrolyte Interphase of Silicon/Carbon Anodes for Lithium Storage
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DOI：10.1002/cey2.70302.png)
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Abstract
En 中文
A durable solid electrolyte interphase (SEI) is essential to mitigating the mechanical fracture and interfacial instability of silicon anodes in view of strong electrochemical-mechanical coupling. In this work, a uniform Li2O layer was accurately deposited on the Si/C composites to regulate the growth characteristics of SEI. By homogenizing the interfacial lithium distribution and inducing directed reduction of fluorine-containing species, the pre-constructed Li2O protective barrier drives the formation of an inorganic integrated hybrid SEI with Li2O/LiF as the main component. This inorganic-rich SEI can significantly optimize the uniformity of lithium flux distribution and regional coordination of expansion stress. Meanwhile, the modified samples exhibited greater mechanical strength and faster Li+ diffusion kinetics, which alleviates the accumulation of local diffusion stress and promotes efficient Li+ transport at the electrode/electrolyte interface. More importantly, Li2O-derived hybrid SEI simultaneously provides effective electrolyte isolation and enhanced mechanical properties, thereby enabling the fundamental inhibition of the sustained decomposition of the electrolyte caused by SEI fragmentation. As a result, the Li2O-modified silicon anode shows an increase of 17.7% in initial Coulombic efficiency (ICE) compared with the original sample (65.3%), along with good cycle stability and rate capability (866 mAh g−1 at 4 A g−1). The effectiveness of the Li2O-rich artificial SEI is further verified in a full cell using LiFePO4 cathode. It is believed that the Li2O-derived multifunctional protective interface inhibits lithium-flux blockage and stress accumulation, offering a robust interfacial strategy for high-capacity Si-based anodes in practical applications.
Keywords:
atomic layer deposition
Li2O layer
lithium-ion batteries
silicon/carbon anode
solid electrolyte interphase
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