Reduced‐Graphene‐Oxide‐Guided Directional Growth of Planar Lithium Layers

Abstract

Rechargeable lithium (Li) metal batteries hold great promise for revolutionizing current energy‐storage technologies. However, the uncontrollable growth of lithium dendrites impedes the service of Li anodes in high energy and safety batteries. There are numerous studies on Li anodes, yet little attention has been paid to the intrinsic electrocrystallization characteristics of Li metal and their underlying mechanisms. Herein, a guided growth of planar Li layers, instead of random Li dendrites, is achieved on self‐assembled reduced graphene oxide (rGO). In situ optical observation is performed to monitor the morphology evolution of such a planar Li layer. Moreover, the underlying mechanism during electrodeposition/stripping is revealed using ab initio molecular dynamics simulations. The combined experiment and simulation results show that when Li atoms are deposited on rGO, each layer of Li atoms grows along (110) crystallographic plane of the Li crystals because of the fine in‐plane lattice matching between Li and the rGO substrate, resulting in planar Li deposition. With this specific topographic characteristic, a highly flexible lithium–sulfur (Li–S) full cell with rGO‐guided planar Li layers as the anode exhibits stable cycling performance and high specific energy and power densities. This work enriches the fundamental understanding of Li electrocrystallization without dendrites and provides guidance for practical applications.

Controlling electrochemical growth of metallic zinc electrodes: Toward affordable rechargeable energy storage systems

“…The metal oxides are reduced to their elemental forms and act as a heterogeneous epitaxial substrate for the Zn electrodeposition. Analogous concept of substrate-induced heteroepitaxy has also been reported for Li metal (142). Even without an epitaxial substrate, metal electrodeposits were found to exhibit some degree of texturing behaviors depending on overpotential as reported in early studies (143,144).…”

Polysiloxane Cross‐Linked Mechanically Stable MXene‐Based Lithium Host for Ultrastable Lithium Metal Anodes with Ultrahigh Current Densities and Capacities

“…To the best of our knowledge, the long cycling stability (3000 h) at such a high current density (20 mA cm −2 ) and areal capacity (10 mAh cm −2 ) of the Li@C 0.5 ‐MXene/AgNW anode is superior to all previously reported Li composite anodes (Figure 4c; Table S2, Supporting Information). [ 9,10,32,40,42,46,49,60–77 ] It also outperforms all Li metal anodes stabilized by other strategies (Table S3, Supporting Information), [ 15,16,20,21,78–86 ] such as SEI layer modification, [ 15,16,78–82 ] separator modification, [ 20,21 ] and electrolyte modification. [ 83–86 ] Moreover, similar to most previously published works, our Li@C 0.5 ‐MXene/AgNW composite anode exhibited better cycling stability in ether based electrolyte than that in carbonate based electrolytes (Figure S8, Supporting Information).…”

Rechargeable Aqueous Zinc‐Ion Batteries with Mild Electrolytes: A Comprehensive Review

“…The researchers also concluded the crystallographic, surface texturing, and electrochemical criteria for the achievement of this reversible epitaxial electro‐deposition. Almost at the same time, Li and Wei et al . reported the similar impacts of graphene on Li plating, confirming the wide applicability of this pathway toward energy‐dense metal batteries (Figure e–q).…”