Lithium is regarded as an ideal anode for next-generation Li metal batteries (LMB) as it exhibits extraordinarily high theoretical capacity and the lowest electrochemical potential among all anode candidates. However, safety concerns and poor cycling stability of Li induced by uncontrollable dendrite growth and severe side reactions impede its practical application for LMB. Although various strategies for fabricating Li anodes have been suggested, developing high-rate LMB remains a significant challenge. To address this challenge, the use of a 3D porous Li–Si alloy-type interfacial framework (LSIF) created via a “self-discharge” mechanism with the aid of an electrolyte is proposed here. Exploiting the in situ spontaneous prelithiation, lithiophilic Li₁₅Si₄ particles are homogenously arranged to build porous 3D LSIF. The balanced ionic/electronic conducting LSIF serves as a stable Li host, helping to suppress dendrite growth and volume expansion during cycling. The LSIF@Li anode possesses a strong affinity toward Li, rapid Li diffusion kinetics, and low nucleation/diffusion barriers. Moreover, the LSIF@Li symmetric cells are capable of stable cycling (over 1000 cycles) even at an ultrahigh current density (15 mA cm^–2). When paired with LiNi_0.5Co_0.2Mn_0.3O₂ or LiFePO₄, LSIF@Li full cells show improved rate capability and long-term cycling stability (≈2000 cycles) at 10 C.

中文翻译：

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多孔亲锂锂硅合金型界面骨架通过自放电机制实现稳定的锂金属负极

锂被认为是下一代锂金属电池 (LMB) 的理想负极，因为它在所有候选负极中表现出极高的理论容量和最低的电化学电位。然而，由不可控的枝晶生长和严重的副反应引起的锂的安全问题和较差的循环稳定性阻碍了其在 LMB 中的实际应用。尽管已经提出了各种制造锂负极的策略，但开发高倍率 LMB 仍然是一个重大挑战。为了应对这一挑战，本文提出了在电解质的帮助下通过“自放电”机制创建的 3D 多孔 Li-Si 合金型界面框架 (LSIF)。利用原位自发预锂化，亲锂 Li ₁₅ Si ₄粒子均匀排列以构建多孔 3D LSIF。平衡的离子/电子导电 LSIF 作为稳定的锂主体，有助于抑制循环过程中的枝晶生长和体积膨胀。LSIF@Li 负极对锂有很强的亲和力、快速的锂扩散动力学和低成核/扩散势垒。此外，即使在超高电流密度（15 mA cm ^–2）下，LSIF@Li 对称电池也能够稳定循环（超过 1000 次循环）。当与 LiNi _0.5 Co _0.2 Mn _0.3 O ₂或 LiFePO ₄配对时，LSIF@Li 全电池在 10 C 下显示出更高的倍率性能和长期循环稳定性（≈2000 次循环）。