Abstract

In this work, a 3D lithiophilic carbon cloth (CC)/ZnO nanorod arrays skeleton and an Li 3 N-rich SEI layer induced by the Mg 3 N 2 -containin electrolyte are co-designed to achieve stable Li metal anode. • The ZnO nanorod arrays is applied to improve the wettability between carbon cloth and molten Li to achieve uniform Li absorption. • High lithiophilic LiZn alloy enforces a uniform Li deposition within the 3D framework. • Li 3 N-rich SEI layer insures a low Li + diffusion energy barrier and inhibits the interfacial side reactions. • The as-prepared composite Li anode offers a long lifespan even at 5 mA cm -2 or 15 mAh cm -2 . Lithium (Li) metal anode offers highest theoretical-specific-capacity among all typical anodes, yet its further utilization is significantly suppressed due to a series of critical challenges, such as uncontrolled Li dendrite growth, continuous side reactions, and unlimited volume variation. In this work, a 3D lithiophilic nature carbon cloth (CC)/ZnO nanorod arrays skeleton and an Li 3 N-rich SEI layer induced by the Mg 3 N 2 -containin electrolyte are co-designed to guide homogenous Li deposition. It is revealed that ZnO nanorods are converted into highly lithiophilic LiZn alloy to induce homogeneous Li deposition within the skeleton and optimize the Li + flux. In addition, the Mg 3 N 2 -containing electrolyte derives an Li 3 N-rich SEI and abundant Mg lithiophilic seeds on the surface, thus reducing the diffusion barrier and deposition barrier. As a result, the CC-ZnO-Mg 3 N 2 /Li anode can deliver a high-capacity of 2205 mA h g −1 , and it also shows a lower nucleation overpotential and a long-running lifespan even at an ultrahigh current density (5 mA cm −2 , 1000 cycles) or an ultrahigh areal capacity (15 mA h cm −2 , >1000 h). In addition, the as-assembled LiFePO 4 ||CC-ZnO-Mg 3 N 2 /Li and LiNi 0.8 Co 0.1 Mn 0.1 O 2 (4.4 mA h cm −2 )||CC-ZnO-Mg 3 N 2 /Li full cells present the improved cycling stability and rate performances. This work gives a new sight to design stable Li composite anode and highlights the critical role of the interfacial stability toward cycling properties of composite Li metal anode.

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