Lithiophilic-lithiophobic gradient interfacial layer for a highly stable lithium metal anode

Huimin Zhang,Hai Ming,Jingyi Qiu,Gaoping Cao,Yan Zhao,Xiaobin Liao,Lin Lu,Xiayu Zhu,Yusheng Yang,Meng Li,Yaqin Huang,Yu Xiang,Yuepeng Guan,Wenfeng Zhang,Hao Zhang,Liqiang Mai

doi:10.1038/s41467-018-06126-z

Abstract

The long-standing issue of lithium dendrite growth during repeated deposition or dissolution processes hinders the practical use of lithium-metal anodes for high-energy density batteries. Here, we demonstrate a promising lithiophilic–lithiophobic gradient interfacial layer strategy in which the bottom lithiophilic zinc oxide/carbon nanotube sublayer tightly anchors the whole layer onto the lithium foil, facilitating the formation of a stable solid electrolyte interphase, and prevents the formation of an intermediate mossy lithium corrosion layer. Together with the top lithiophobic carbon nanotube sublayer, this gradient interfacial layer can effectively suppress dendrite growth and ensure ultralong-term stable lithium stripping/plating. This strategy is further demonstrated to provide substantially improved cycle performance in copper current collector, 10 cm2 pouch cell and lithium–sulfur batteries, which, coupled with a simple fabrication process and wide applicability in various materials for lithium-metal protection, makes the lithiophilic–lithiophobic gradient interfacial layer a favored strategy for next-generation lithium-metal batteries.

Highlights

The long-standing issue of lithium dendrite growth during repeated deposition or dissolution processes hinders the practical use of lithium-metal anodes for high-energy density batteries
In the last ten years, the soaring interest in Li–sulfur and Li–air batteries has intensified these efforts of suppressing dendrite growth, and the associated research can be classified into five categories[17,18,19]: (i) replacing Li metal with a LiX alloy (X = Al, Si, C, etc.) to alleviate the concerns of dendrite growth, (ii) designing high-modulus solid electrolytes to suppress dendrite penetration[20,21,22], (iii) optimizing electrolyte components or developing stable modified interfaces to reinforce solid electrolyte interphase (SEI) formation and prevent dendrite propagation[13,23,24], (iv) manipulating the nanoarchitectures of the Li-metal anode and minimizing electrode dimension variation by stable hosts, skeleton structures, or metal current collectors[15,25,26,27,28,29], and (v) constructing a robust and electrochemically stable upper interfacial layer for Li-metal anodes[10,30,31,32,33,34,35,36]
We have found that even the best interfacial layer, i.e., lithiophobic carbon nanotubes (CNT), failed to effectively regulate Li deposits over the long term because a mossy Li layer tended to form underneath the CNT interfacial layer

Summary

Introduction

The long-standing issue of lithium dendrite growth during repeated deposition or dissolution processes hinders the practical use of lithium-metal anodes for high-energy density batteries. The gradient interfacial layer can suppress dendrite growth effectively and ensure ultralong-term stable Li stripping/plating even at a high current density with a high Li capacity, facilitating the integration of various advantages from Li protection strategies using the reported carbon materials. This strategy is further demonstrated to be successful in copper (Cu) current collector, 10 cm[2] pouch cell and Li–sulfur (Li–S) batteries. This lithiophilic–lithiophobic gradient strategy is applicable to carbon materials such as CNT and can accommodate other materials for Li anode modification such as incorporation of electrospun fibers

Methods

Results

Conclusion