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Boosting stable lithium deposition via Li3N-Enriched inorganic SEI induced by a polycationic polymer layer
Cao, Wenzhu1,2; Chen, Weimin1; Lai, Zhenghan1; Chen, Hong1; Tian, Du1; Wang, Liang3; Yu, Faquan1
2025
摘要Lithium (Li) metal is a promising anode material for future high-energy rechargeable batteries due to its remarkable properties. Nevertheless, excess Li in traditional lithium metal anodes (LMAs) reduces the energy density of batteries and increases safety risks. Electrochemical pre-lithiation is an effective technique for regulating the lithium content of the anodes. However, Cu foil or other non-Li based substrates used for pre-lithiation often have inhomogeneous surfaces and high nucleation barrier, leading to uneven tip deposition of lithium metal and fragile SEI. Herein, we have designed an interfacial layer composed of nano-Si particles and cationic polymer (poly (diallyldimethylammonium chloride)) (denoted as Si@PDDA) to induce the formation of Li3N-rich inorganic SEI and regulate the homogeneous plating/stripping of lithium. The uniformly dispersed nano-Si particles can decrease the Li+ nucleation overpotential through alloying reaction with lithium. The surface of Si nano-particles modified by PDDA contains numerous cationic sites, providing an electrostatic shielding layer to seeding the growth of Li metal and inhibiting dendrites formation. More promisingly, PDDA adsorbs electrolyte anions while transporting Li+, significantly accelerating the decomposition kinetics of inorganic salts within the electrolyte. Therefore, a SEI film rich in Li3N was formed on the anodes, ensuring the excellent interfacial stability and electrochemical cycling performance of LMAs. The symmetrical cells exhibit a cycle life of 900 h at 1 mA cm(-2). Moreover, the practical full cells operate at a low negative/positive (N/P) capacity ratio (similar to 3) for over 160 cycles.
关键词Cationic polymer poly Nano-Si particles Li-Si alloy Li3N SEI
DOI10.1016/j.jcis.2024.07.246
发表期刊JOURNAL OF COLLOID AND INTERFACE SCIENCE
ISSN0021-9797
卷号677页码:481-490
通讯作者Chen, Weimin(wmchen@wit.edu.cn) ; Wang, Liang(wangliang@cigit.ac.cn) ; Yu, Faquan(fyu@wit.edu.cn)
收录类别SCI
WOS记录号WOS:001289613600001
语种英语