Curvature-induced strain to realize differential lithiophilicity for selective lithium deposition and stable lithium anode

Abstract

Regulating the lithiophilicity of three-dimensional (3D) lithium hosts is crucial for improving lithium deposition and suppressing dendrite growth. However, previous research has mainly focused on varying lithiophilic components, and the impact of geometric structures induced strain remains poorly understood. Herein, we present a novel curvature-induced strain engineering approach to regulate lithiophilicity and deposition kinetics of lithium in lightweight 3D tubular carbon hosts. A hollow carbon fiber with bilateral growth of MnO2 nanosheet arrays both inside and outside the tubes (MnO2@HCFC) have been successfully synthesized. Theoretical calculations and experiments confirm that the MnO2 layers inside and outside the hollow carbon fiber tube undergo compressive and tensile strain, respectively. The curvatures induced strain modifies the O2p band center of the lithiophilic MnO2 layer, enabling the regulation of lithiophilicity and preferential and uniform lithium deposition within the carbon fiber tubes. The MnO2@HCFC framework exhibits excellent lithium affinity and uniform Li+ flux distribution, as evidenced by visualization techniques and COMSOL simulations, enabling dendrite-free lithium deposition. The Li-MnO2@HCFC||LiCoO2 full cell retains 85.7 % of its capacity after 400 cycles at 0.5 C with a high LiCoO2 loading of 10.3 mg cm-2. The optimized lithium anode pouch cell exhibits robust cycle stability under harsh conditions. This work offers new insight into the design of 3D lithium hosts to enhance the performance of lithium anodes through curvature-induced strain engineering.