Natural SEI-Inspired Dual-Protective Layers via Atomic/Molecular Layer Deposition for Long-Life Metallic Lithium Anode

Abstract

The solid electrolyte interphase (SEI) layer is one of the key factors for Li metal anode affecting the Li-deposition behavior and electrochemical performances. However, the fabrication of artificial SEI layers with precisely controlled composition, thickness, and mechanical properties is still challenging and difficult to be realized. In this study, we demonstrate an SEI-inspired dual protective layer for Li metal anode with highly controllable structures and robust mechanical properties (the organic alucone as the outer layer and inorganic Al 2 O 3 as the inner layer), which is deposited by atomic layer deposition (ALD) and molecular layer deposition (MLD) techniques. The dual-layer protected Li anode displays significantly enhanced electrochemical performances, suppressed mossy/dead Li formation, and robust properties during the plating/stripping process. It is believed that our design of dual-layer protected Li metal anode by ALD and MLD opens up new opportunities for the realization of next-generation high-energy-density Li metal batteries.

Revealing and Elucidating ALD‐Derived Control of Lithium Plating Microstructure

“…To address the fallibilities of lithium metal, numerous strategies have been employed, ranging from designing electrolytes to reduce the number of side reactions between lithium and the electrolyte, [11][12][13][14] engineering hosts that accommodate and control the expansion of lithium, [15][16][17][18][19][20][21] and, in some very recent cases, to incorporating artificial SEIs that passivate the interface between lithium metal and the electrolyte. [22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37] Of all the modern strategies employed to passivate lithium metal, artificial SEIs positioned at the Li-electrolyte interface have shown some of the most promising results. Materials such as polymers, [25][26][27] inorganic metal oxides, [27][28][29] inorganic nitrides, [30] fluorides, [31][32][33] nanodiamond, [34] and hybrid structures [35,36] have been applied as interfacial layers, and for the most part, they support uniform plating and stripping of lithium by passivating the reactive Li surface against the electrolyte.…”

“…[22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37] Of all the modern strategies employed to passivate lithium metal, artificial SEIs positioned at the Li-electrolyte interface have shown some of the most promising results. Materials such as polymers, [25][26][27] inorganic metal oxides, [27][28][29] inorganic nitrides, [30] fluorides, [31][32][33] nanodiamond, [34] and hybrid structures [35,36] have been applied as interfacial layers, and for the most part, they support uniform plating and stripping of lithium by passivating the reactive Li surface against the electrolyte. In the formation of artificial SEIs, the use of techniques that ensure conformality at the interface is key, and as a result, there is a predilection for the use of atomic layer deposition (ALD) and molecular layer deposition (MLD).…”

“…To address the fallibilities of lithium metal, numerous strategies have been employed, ranging from designing electrolytes to reduce the number of side reactions between lithium and the electrolyte, [ 11–14 ] engineering hosts that accommodate and control the expansion of lithium, [ 15–21 ] and, in some very recent cases, to incorporating artificial SEIs that passivate the interface between lithium metal and the electrolyte. [ 22–37 ]…”

CO2-based atomic/molecular layer deposition of lithium ethylene carbonate thin films

“…2,4 It is clear from numerous studies that an articially pre-fabricated SEI could improve battery performance by preventing cracks and stopping the consumption of the electrolyte and Li-ions. [5][6][7][8][9][10][11][12][13][14][15][16] An articial SEI could also help prevent damage caused by mechanical stress and by volume expansion during (de)insertion of Li-ions, but this feature is dependent on the cell chemistry.…”

A New Strategy of Constructing a Highly Fluorinated Solid‐Electrolyte Interface towards High‐Performance Lithium Anode

“…The well‐designed dual‐layered SEI is able to protect Li metal and suppress Li‐dendrite growth. [ 23 ]…”