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Metallurgical refractory lining-guided inorganic binder for stable lithium storage in silicon microparticle anodes
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DOI：10.1039/D5EE03194J.png)
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Abstract
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Silicon is a promising anode material for next-generation lithium-ion batteries (LIBs); offering a significantly higher theoretical capacity than graphite. While nano-silicon excels; its high cost limits practicality; making silicon microparticles (μSi) a more economical; scalable alternative. However; μSi anodes are hindered by substantial capacity degradation; resulting from the over 300% volume expansion during cycling. This study introduces an aluminum dihydrogen phosphate (Al(H2PO4)3; AHP) binder system; designed based on principles of refractory chemistry; which effectively mitigates interfacial instability and mechanical failures in μSi anodes. The water-soluble AHP binder forms a uniform electrode through in situ dehydration condensation; creating a covalently cross-linked inorganic network. This high-modulus cross-linked network restricts the expansion of μSi particles during cycling; thereby preserving electrode integrity. As a result; μSi anodes incorporating the AHP binder exhibit exceptional cyclability; retaining a capacity of 1300.4 mAh g-1 after 200 cycles at 0.5 A g-1; alongside impressive rate capabilities of 936.4 mAh g-1 and 769.1 mAh g-1 at 4 A g-1 and 5 A g-1; respectively. Additionally; the AHP binder demonstrates superior compatibility with lithium iron phosphate (LiFePO4; LFP) cathodes. This work establishes inorganic binders as a practical and economical solution for high-performance μSi anodes; enhancing LIBs energy density and lifespan.
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