Designing 3D Anode Based on Pore‐Size‐Dependent Li Deposition Behavior for Reversible Li‐Free All‐Solid‐State Batteries

Abstract

Li‐free all‐solid‐state batteries can achieve high energy density and safety. However, separation of the current collector/solid electrolyte interface during Li deposition increases interfacial resistance, which deteriorates safety and reversibility. In this study, a reversible 3D porous anode is designed based on Li deposition behavior that depends on the pore size of the anode. More Li deposits are accommodated within the smaller pores of the Li hosting anode composed of Ni particles with a granular piling structure; this implies the Li movement into the anode is achieved via diffusional Coble creep. Surface modification of Ni with a carbon coating layer and Ag nanoparticles further increases the Li hosting capacity and enables Li deposition without anode/solid electrolyte interface separation. A Li‐free all‐solid‐state full cell with a LiNi0.8Mn0.1Co0.1O2 cathode shows an areal capacity of 2 mAh cm−2 for retaining a Coulombic efficiency of 99.46% for 100 cycles at 30 °C.

Anode-less all-solid-state batteries: recent advances and future outlook

“…Park et al adopted nickel powder coated with carbon and silver for the protective layer [37]. At the same time, they regulated the internal voids in terms of size by packing the nickel particles with controlled sizes and distributions, which led the authors to learn that the smaller voids result in more uniform penetration of Li metal via the coble creep mechanism.…”

Lithium–silver alloys in anode-less batteries: comparison in liquid- and solid-electrolytes

“…A sharp voltage dip during the plating process of the LE-based cell corresponded to the nucleation overpotential required for the formation of Li–Ag alloys with sufficiently large nuclei for the growth of Li deposits. 14,15 Conversely, it is noteworthy that the SE-based cell did not exhibit such a sharp voltage dip, suggesting a different Li electrodeposition mechanism 16–19 in LE- and SE-based cells. Considering the smaller voltage dips but larger Li growth plateaus for the SE-based cell compared to the LE-based cell, the kinetics of Li diffusion appear to outweigh the thermodynamics of Li electrodeposition in the SE-based cell.…”

Two-dimensional LiTi2(PO4)3 flakes for enhanced lithium ions battery anode

“…Currently, the graphite anode is the priority for LIBs towards the commercialization, which is cost-effective and stable as well as the abundant reserves [ [6] , [7] , [8] ]. Unfortunately, the inherent disadvantage associating with graphite anode is low Li + intercalation potential (0.1 V vs. Li + /Li), which probably leads to the deposition of metal lithium, giving rise to safety issues and poor rate performance [ [9] , [10] , [11] ]. Alternatively, the promising insertion host materials, such as TiO 2 , Li 4 Ti 5 O 12 , LiCrTiO 4 and LiTi 2 (PO 4 ) 3 (LTP) have been recommended as the potential anode instead of graphite [ [12] , [13] , [14] , [15] , [16] ].…”