3D-Printed Porous GO Framework Enabling Dendrite-Free Lithium-Metal Anodes

Abstract

Although lithium-metal anode is regarded as the most promising candidate for high-energy-density batteries, the uncontrollable Li dendrite growth and large volumetric change have severely inhibited its practical application. Herein, a three-dimensional (3D)-printed graphene oxide framework was constructed as a lithium-metal host to modulate the plating behavior of Li+ on the interfaces. Owing to the specially designed architecture, the 3D-printed GO framework can effectively reduce the local current density and supply large space for the accommodation of Li to buffer the volume change. As a result, the 3D-GO@Li anode enables a dendrite-free Li plating/stripping with a small overpotential of 9 mV and a long-term cycling stability of 1600 h at 1 mA cm–2. Moreover, the stable 3D-GO@Li anode is further corroborated via a full battery with a LiFePO4 cathode with a superior long cycle lifespan and capacity retention in comparison to the pristine Li anode. This work would pave a promising way for 3D printing technology to construct high-energy-density energy storage devices.

Extrusion 3D Printing of Patterned Cu Current Collectors for Advanced Lithium Metal Anodes

“…Additionally, the huge storage space provided by the 3D pattern can mitigate the typical volume deformation of the lithium anode that is responsible for cycling instability and severe cell failure. Similar improvements related to the porous framework have been also observed for other 3D printed networks, as, for example, in case of graphite‐based skeletons for Li metal anodes [28] …”

“…Similar improvements related to the porous framework have been also observed for other 3D printed networks, as, for example, in case of graphite-based skeletons for Li metal anodes. [28]…”

Lightweight 3D Lithiophilic Graphene Aerogel Current Collectors for Lithium Metal Anodes

“…The CE of the half cell with carbon nanotubes acting as the 3D current collector remained at 90% over 150 cycles at 1 mA cm −2 [44]. The 3D-printed graphene oxide framework reduced the local current density and supplied space for the deposition of Li, enabling a long-term cycling stability of 1600 h at 1 mA cm −2 [45]. Despite the good modification effect, poor mechanical stability will accelerate the failure of the battery.…”

Fast rate lithium metal batteries with long lifespan enabled by graphene oxide confinement

“…41,44 The Li adsorption is also demonstrated to strengthen by increased Li metal coverages due to Li metal forming bonds with both oxygen and carbon of the GO layer. 44 In addition to the lack of the confinement effect, many prior works on GO 28,[57][58][59][60][61][62][63][64][65] are limited due to multi-step and difficult synthetic procedure, high mass ratio of GO, capacity loss of the Li metal anode, and relatively poor lifespan of the developed LMBs are among some of the issues with the composite design. The confinement effect is most effective if there is a strong chemical interaction between the GO layer and the separator or Li metal anode associated with parallelly-aligned GO layers.…”

“…41,44 The Li adsorption is also demonstrated to strengthen by increased Li metal coverages due to Li metal forming bonds with both oxygen and carbon of the GO layer. 44 In addition to the lack of the confinement effect, many prior works on GO 28,[57][58][59][60][61][62][63][64][65] Here, we propose a new strategy to suppress the dendritic growth of Li by confinement of Li at the interface with the GO layer. This is achieved by a thin, dense coating of parallelly-aligned GO layers at the interface with Li metal ensuring an effective confinement effect between the GO layer and Li metal surface.…”