Electroless plating of tin on copper foil (2-D) and foams (3-D) was used to create carbon- and binder-free thin films for solid electrolyte interphase (SEI) property investigation. When electrochemically cycled vs lithium metal in coin cells, the foam electrodes exhibited better cycling performance than the planar electrodes due to electrode curvature. The effect of the additive/cosolvent fluoroethylene carbonate (FEC) was found to drastically improve the capacity retention and Coulombic efficiency of the cells. The additive amount of 2% FEC is enough to derive the benefits in the cells at a slow (C/9) cycling rate. The interfacial properties of Sn thin film electrodes in electrolyte with/without FEC additive were investigated using in situ electrochemical quartz crystal microbalance with dissipation (EQCM-D). The processes of the decomposition of the electrolyte on the electrode surface and Li alloying/dealloying with Sn were characterized quantitatively by surface mass change at the molecular level. FEC-containing electrolytes deposited less than electrolyte without FEC on the initial reduction sweep, yet increased the overall thickness/mass of SEI after several cyclic voltammetry cycles. EQCM-D studies demonstrate that the mass accumulated per mole of electrons (mpe) was varied in different voltage ranges, which reveals that the reduction products of the electrolyte with/without FEC are different.
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http://dx.doi.org/10.1021/am508593s | DOI Listing |
Chem Sci
January 2025
School of Materials and Energy, University of Electronic Science and Technology of China Chengdu 611731 China
Silicon (Si) is considered a promising anode material for next-generation lithium-ion batteries due to its high theoretical specific capacity and earth-abundancy. However, challenges such as significant volume expansion, unstable solid electrolyte interphase (SEI) formation in incompatible electrolytes, and slow lithium-ion transport lead to its poor cycling and rate performance. In this work, it is demonstrated that superior cyclability and rate capability of Si anodes can be achieved using ethyl fluoroacetate (EFA) and fluoroethylene carbonate (FEC) solvents with low binding energy with Li but with sufficiently high relative dielectric constants.
View Article and Find Full Text PDFACS Appl Mater Interfaces
January 2025
Research Center of Nano Science and Technology, College of Sciences, Shanghai University, Shanghai 200444, China.
The interfacial reaction of a silicon anode is very complex, which is closely related with the electrolyte components and surface elements' chemical status of the Si anode. It is crucial to elucidate the formation mechanism of the solid electrolyte interphase (SEI) on the silicon anode, which promotes the development of a stable SEI. However, the interface reaction mechanism on the silicon surface is closely related to the surface components.
View Article and Find Full Text PDFNanomicro Lett
December 2024
State Key Laboratory of Space Power-Sources, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin, 150001, People's Republic of China.
Micrometer-sized silicon oxide (SiO) anodes encounter challenges in large-scale applications due to significant volume expansion during the alloy/de-alloy process. Herein, an innovative deep eutectic electrolyte derived from succinonitrile is introduced to enhance the cycling stability of SiO anodes. Density functional theory calculations validate a robust ion-dipole interaction between lithium ions (Li) and succinonitrile (SN).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
State Key Laboratory of Material Processing and Die & Mould Technology, Institute for Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei, 430074, China.
Sulfurized polyacrylonitrile (SPAN) presents an opportunity to replace elemental sulfur as a "shuttle-free" cathode for secondary Li-S batteries, which can be an ideal choice for stationary energy storage due to its abundance, low cost, and sustainability. The electrolyte options for the state-of-the-art SPAN batteries have been limited to the flammable carbonate and ether ones, which raises safety concerns. Here, we explored the use of a non-flammable acetonitrile (AN) electrolyte for SPAN battery for the first time and identified the irreversible cleavage of C-S bonds of SPAN as the main reason for the failure of SPAN in AN electrolyte.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2024
i-Lab, iVacuum interconnected Nanotech Workstation (Nano-X), iSuzhou Institute of Nano-Tech and Nano-Bionics (SINANO), Chinese Academy of Sciences, Suzhou, Jiangsu, 215123, China.
Room-temperature sodium-sulfur (RT Na-S) batteries has attracted growing attentions in large-scale energy storage technology, while the serious shuttle effect and interface side reaction limit its practical application. Despite fluoroethylene carbonate (FEC) has been widely used as an electrolyte additive or co-solvent to facilitate the optimization of electrode-electrolyte interphase in RT Na-S batteries, its crucial influence and mechanism have not been clearly understood. Herein, we deeply reveal the two-steps cathode-electrolyte interphase (CEI) formation by using FEC as the exclusive electrolyte solvent.
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