From Dendrites to Hemispheres: Changing Lithium Deposition by Highly Ordered Charge Transfer Channels

Abstract

Metallic lithium as an anode is an ultimate ideal for rechargeable lithium batteries with high energy density such as lithium–oxygen batteries and lithium–sulfur batteries. However, the excess reactivity and asymmetrical dissolution–deposition of the metallic lithium anode make it impossible to support a stable long charge–discharge cycling. To protect the metallic lithium anode, apparently it needs to adjust the dissolution and deposition of lithium ions, but more essentially, it should reasonably change the distribution and transport of electrons on the surface and interface of the metallic lithium. In this work, anodic aluminum oxide (AAO) membranes are used to build highly ordered channels on the lithium anode surface in which lithium ions can transfer in the channels and electrons can be transported by the lithiation reaction of alumina with an oxygen vacancy-involved process. As a result, the cyclic reaction actually is partially transferred to the AAO surface, and lithium deposition occurs there as a hemispherical appearance but not as dendrites. Meanwhile, the highly ordered characteristics provide a physical effect to make the deposited lithium hemispheres a uniform distribution on the AAO surface. The AAO-regulated lithium anodes could be widely used to improve the cycling performance for metal lithium batteries.

Heterostructured Gel Polymer Electrolyte Enabling Long-Cycle Quasi-Solid-State Lithium Metal Batteries

“…Apparently, this is caused by lithium partially reducing Al 2 O 3 at the interface of both. 1,56 The F 1s spectrum of the lithium electrode and the Li 1s spectrum of GPE-ZIF8-Al 2 O 3 after being cycled are actually very complicated because these spectra could contain the signals of organic salt besides LiF and AlF 3 . However, from the C 1s spectrum of the lithium electrode, it can be found that C−F, CO, C−O, C−H, and C−C bonds appear in the surface of lithium after cycling.…”

“…Metallic lithium has attracted extensive research attention as a promising anode material for rechargeable lithium–metal batteries (RLBs) with a large theoretical specific capacity of 3860 mAh g –1 and low reduction potential (−3.04 V vs standard hydrogen electrode). − It is expected to build RLBs with high energy and power density to meet the increasing demands of future electronic equipment and electric vehicles. However, the lithium anode tends to trigger parasite reactions with the traditional organic liquid electrolyte due to its excessive reaction activity during the charge/discharge process .…”

“…As pointed out in the previous studies, the fluorides, especially LiF and AlF 3 , are beneficial for lowering the diffusion energy barrier to ensure a fast diffusion rate and strengthen the mechanical properties of the SEI film during cycling. , A noteworthy result is the signal of AlO x in GPE-ZIF8-Al 2 O 3 after cycling. Apparently, this is caused by lithium partially reducing Al 2 O 3 at the interface of both. , The F 1s spectrum of the lithium electrode and the Li 1s spectrum of GPE-ZIF8-Al 2 O 3 after being cycled are actually very complicated because these spectra could contain the signals of organic salt besides LiF and AlF 3 . However, from the C 1s spectrum of the lithium electrode, it can be found that C–F, CO, C–O, C–H, and C–C bonds appear in the surface of lithium after cycling.…”

A Critical Review on the Recycling Strategy of Lithium Iron Phosphate from Electric Vehicles

“…[31][32][33] At present, the presence of SEI has been detected on the surface of several common anode materials such as metal lithium, [34,35] graphite [36] and silicon. [37][38][39] Figure 3a shows the relative electron energies of the anode, electrolyte and cathode for the thermodynamically stable redox pair in the LIBs. [40] If the electrochemical potentials of the anode (μA) are higher than the lowest unoccupied molecular orbital (LUMO) energy or the electrochemical potentials of the cathode (μC) are lower than the highest occupied molecular orbital (HOMO) energy, the electrode materials will undergo a redox reaction with the electrolyte to form SEI.…”

A lithiophilic AlN-modified copper layer for high-performance lithium metal anodes

“…Utilizing the porous composite electrode with large specic surface areas, 15,16 increasing lithium deposition sites and reducing current density could realize the uniform lithium deposition, but the volumetric energy density of the electrode is sacriced, and large specic surface area will lead to more side reactions. Besides, protective coating layers composed of polymers, [17][18][19][20] inorganic materials [21][22][23] and their mixtures [24][25][26][27] are applied to suppress the lithium dendrites and improve the brittleness of SEI, but the transport kinetics of lithium ions in the modied layer still needs to be increased to alleviate the space charge layer. Therefore, it is essential to construct fast ion transport channels in the protective coating layer to ensure the rapid transport of lithium ions particularly.…”