A Fishing‐Net‐Like 3D Host for Robust and Ultrahigh‐Rate Lithium Metal Anodes

Abstract

Constructing an architectural host is demonstrated to be an effective strategy for long‐life lithium metal anodes (LMAs). Herein, an integrated 3D host for stable and ultrahigh‐rate LMAs is developed by a binary highly conductive network of 2D reduced graphene oxide (rGO) and 1D carbon nanofibers (CNF) anchored with 0D ultrasmall MgZnO nanoparticles (MgZnO/CNF‐rGO). A facile net‐fishing strategy is proposed to combine the rGO nanosheets with free‐standing CNF matrix as interconnected paths for fast electron transport. Notably, serving as Li nucleation sites, the superlithiophilic MgZnO nanoparticles are uniformly distributed and tightly contacted with the conductive matrix without agglomeration due to the rGO confinement. Such a delicate nanoscale combination guarantees the effective transportation and uniform deposition of Li‐ions in the inner surface of the host. The symmetric cell of Li@MgZnO/CNF‐rGO exhibits a long lifespan above 1450 cycles under an ultrahigh current density of 50 mA cm−2 with an areal capacity of 1.0 mAh cm−2. Impressively, it also delivers a high reversible capacity of 10 mAh cm−2 at 50 mA cm−2. This work offers an avenue to promise the prospect for practical LMAs working under high rates and capacities.

In situ tailoring solid electrolyte interphase of three‐dimensional Li metal electrode for enhanced Coulombic efficiency

“…Among various strategies attempted to tackle the challenges mentioned above, 7–12 constructing a three‐dimensional (3D) current collector is an efficient method to mitigate dendrite growth as the 3D configuration with a high specific surface area and the porous structure can reduce the local current density and accommodate the volume change upon repeated stripping/plating 13,14 . A number of successful demonstrations of uniform Li deposition by adopting the 3D strategy can be found in the literature, such as porous metal‐based foams and 3D carbon‐based frameworks 15–18 . However, the high specific surface area of a 3D host is double‐bladed, as it also leads to an increased interfacial reaction between the Li metal and electrolyte, making the already unstable interface (between Li and existing electrolytes) worse, and serving as a major contributor to the low Coulombic efficiency commonly associated with the 3D configuration 19,20 .…”

In situ tailoring solid electrolyte interphase of three-dimensional Li metal electrode for enhanced Coulombic efficiency

“…[13,14] A number of successful demonstrations of uniform Li deposition by adopting the 3D strategy can be found in the literature, such as porous metalbased foams and 3D carbon-based frameworks. [15][16][17][18] However, the high specific surface area of a 3D host is double-bladed, as it also leads to an increased interfacial reaction between the Li metal and electrolyte, making the already unstable interface (between Li and existing electrolytes) worse, and serving as a major contributor to the low Coulombic efficiency commonly associated with the 3D configuration. [19,20] To improve the CE, constructing artificial solid-electrolyte interphase (SEI) to reduce the irreversible reaction between electrolyte and lithium metal is a commonly adopted method.…”

Li-Ca Alloy Composite Anode with Ant-Nest-Like Lithiophilic Channels in Carbon Cloth Enabling High-Performance Li Metal Batteries

“…Generally, constructing an architectural host and then infiltrating molten Li metal into a three-dimensional (3D) conductive skeleton to alleviate the volume change is regarded as an effective strategy to enhance the lifespan and stability of Li metal anode [4][5][6][7][8]. Among various 3D conducting skeletons, carbon-based materials are very promising as advanced host of Li metal anode due to the benefits of low density, favorable electrical conductivity, cheap, excellent chemical stability, and robust mechanical strength [9][10][11][12][13].…”