Negatively Charged Holey Titania Nanosheets Added Electrolyte to Realize Dendrite‐Free Lithium Metal Battery

Abstract

growth and unstable solid electrolyte interface (SEI), which leads to low coulombic efficiency, capacity fading, and safety issues. [6][7][8][9][10] To solve these problems, various strategies have been proposed, including electrode engineering, electrolyte design, artificial solid electrolyte layer construction, separator film modification, etc. [11][12][13][14][15][16][17][18] Among all these strategies, the electrolyte modulation and electrode engineering are most effective and widely used. The rational modulation of the electrolyte can promote the robust SEI formation and improves the uniform lithium-ion flux. The related works include the design of high concentration electrolytes, dual-salt/ dual-solvent electrolyte, inorganic additive, organic additive, solid state electrolyte, and so on. [19][20][21][22][23][24][25] The electrode engineering is generally used to suppress the dendritic growth through regulating lithium-ion flux on the anode surface. [26,27] The commonly applied methods include the building of 3D conductive host to decease the local current density and homogenize space charge distribution, and decorating the surface with lithiophilic sites to regulate the uniform lithium nucleation and growth. [28][29][30][31] However, either the electrolyte modulation or electrode design has its own advantages and disadvantages. Electrolyte modulation is simple, but not very effective to regulate the ion flux. Electrode engineering can more effectively regulate lithium-ion flux on the electrode surface, but the process is complicated. Therefore, we are thinking the possibility to combine the merits of these two strategies into one.Considering the simplicity of adding additives into electrolyte, we propose a new method for the rational electrode design through the concept of electrolyte additive. By adding the materials used to construct the 3D electrode into the electrolyte, they will self-assemble into hierarchical structure on the current collector under the electrical field between the cathode and anode. In this case, the electrode modification will be much easier and the homogeneity of the modification on the Li metal anode can also be well controlled, even in large size anodes. However, to realize the proposed idea, several basic requirements should be satisfied: (1) The additives are supposed to be stable for a certain period in the common lithium battery electrolyte; (2) The additives should have charge to move under electric fields to realize self-adaptive electrode surface modification; (3) The Electrolyte modulation and electrode structure design are two common strategies to suppress dendrites growth on Li metal anode. In this work, a self-adaptive electrode construction method to suppress Li dendrites growth is reported, which merges the merits of electrolyte modulation and electrode structure design strategies. In detail, negatively charged titania nanosheets with densely packed nanopores on them are prepared. These holey nanosheets in the electrolyte move spontaneously onto the anode under elec...

Cross-Linked Polymer Composite Electrolyte Incorporated with Waste Seashell Based Nanofiller for Lithium Metal Batteries

“…Similarly, the pristine (PEO and LiClO 4 ) Li|Pristine|LFP provides the discharge capacity of 15 mAh g –1 at 0.1 C. The fabricated full cells are subjected to 0.2, 0.5, and 1 C rates, which deliver the discharge capacities of 140 mAh g –1 , 90 mAh g –1 , and 80 mAh g –1 at 60 °C as shown in Figure b. The incorporated porous Ca­(OH) 2 with higher surface area tends to improve the amorphous nature of the electrolyte, which favors Li-ion transfer, thereby exhibiting good charge/discharge capacity. , In addition, the functionally aligned cross-linked structure (Figure S9) helps to enhance the mobility of the Li ions at a faster rate through the hopping mechanism. It is important to note that the polarization keeps increasing due to the poor interface between the electrodes and electrolyte during charging/discharging.…”

Review of Nanoarrays in Lithium Metal Anodes

“…Similarly, a different approach has been proposed for the construction of negative electrode structures. Luo et al 114 proposed a method for the construction of 3D electrodes using the addition of electrolyte additives. The negatively charged material is added to the electrolyte as an electrolyte additive, and then self-assemble into a hierarchical structure under the influence of an electric field.…”

“…SEM shows that (e) Ti 0.8 Fe 0.1 O 2 nanosheets are densely arranged on a smooth surface, (f) while Ti 0.8 O 2 0.8– nanosheets exhibit a porous structure. Reproduced with permission from ref . Copyright 2023 Wiley.…”

Electrochemically Dealloyed 3D Porous Copper Nanostructure as Anode Current Collector of Li‐Metal Batteries

“…[44] Luo et al conducted phase field simulation to track the Li morphology evolution on different current collectors, and demonstrated that 3D current collector can help suppress Li dendrite growth and promote Li metal deposition by homogenizing Li + flux. [45,46] However, many of these methods are sophisticated with multiple steps and were only demonstrated in small scales such as in coin cells. The scale-up of these methods can be difficult and high-cost.…”