Achieving Uniform Li Deposition and Suppressed Electrolyte Flammability in Li-Metal Batteries via Designing Localized High-Concentration Electrolytes.

The increasing need for energy storage devices with high energy density has led to significant interest in Li-metal batteries (LMBs). However, the use of commercial electrolytes in LMBs is problematic due to their flammability, inadequate performance at low temperatures, and tendency to promote the growth of lithium dendrites and other flaws. This study introduces a localized high-concentration electrolyte (LHCE) that addresses these issues by employing non-flammable electrolyte components and incorporating carefully designed additives to enhance flame retardancy and low-temperature performance. By incorporating additives to optimize the electrolyte, it is possible to attain inorganic-dominated solid electrolyte interphases on both the cathode and anode. This achievement results in a uniform deposition of lithium, as well as the suppression of electrolyte decomposition and cathode deterioration. Consequently, this LHCE achieve over 300 stable cycles for both LiNi0.9Mn0.05Co0.05O2||Li cells and LiCoO2||Li cells, as well as 50 cycles for LiNi0.8Mn0.1Co0.1O2 (NCM811||Li) pouch cells. Furthermore, NCM811||Li cells maintain 84% discharge capacity at -20 °C, in comparison to the capacity at room temperature. The utilization of this electrolyte presents novel perspectives for the safe implementation of LMBs.

Stabilization of LiCoO2 Cathodes in High Voltage Lithium Metal Batteries Through 2-(Trifluoromethyl)Benzamide (2-TFMBA) Electrolyte Additives.

Increasing the charging cutoff voltage of LiCoO2 to 4.6 V is significant for enhancing battery density. However, the practical application of Li‖LiCoO2 batteries with a 4.6 V cutoff voltage faces significant impediments due to the detrimental changes under high voltage. This study presents a novel bifunctional electrolyte additive, 2-(trifluoromethyl)benzamide (2-TFMBA), which is employed to establish a stable and dense cathode-electrolyte interface (CEI). Characterization results reveal that an optimized CEI is achieved through the synergistic effects of the amide groups and trifluoromethyl groups within 2-TFMBA. The resulting CEI not only enhances the structural stability of LiCoO2 but also serves as a high-speed lithium-ion conduction channel, which expedites the insertion and extraction of lithium ions. The Li‖LiCoO2 batteries with 0.5 wt% 2-TFMBA achieves an 84.7% capacity retention rate after enduring 300 cycles at a current rate of 1 C, under a cut-off voltage of 4.6 V. This study provides valuable strategic insights into the stabilization of cathode materials in high-voltage batteries.

Stabilizing Pt Single Atoms through Pt-Se Electron Bridges on Vacancy-enriched Nickel Selenide for Efficient Electrocatalytic Hydrogen Evolution.

Rational design of Pt single-atom catalysts provides a promising strategy to significantly improve the electrocatalytic activity for hydrogen evolution reaction. In this work, we presented a novel and efficient strategy for utilizing the low electron-density region of substrate to effectively trap and confine high electron-density metal atoms. The Pt single-atom catalyst supported by nickel selenide with rich vacancies was prepared via a hydrothermal-impregnation stepwise approach. Through experimental testation and DFT theoretical calculation, we confirm that Pt single atoms are well distributed at cationic vacancies of nickel selenide with loading amount of 3.2 wt. %. Moreover, the atomic Pt combined with the high electronegative Se to form Pt-Se bond as a "bridge" between single atoms and substrate for fast electron translation. This novel catalyst shows an extremely low overpotential of 45 mV at 10 mA cm-2 and an excellent stability over 120 h. Furthermore, the nickel selenide supported Pt SACs exhibits long-term stability for practical application, which maintains a high current density of 390 mA cm-2 over 80 h with a retention of 99 %. This work points a promising direction for designing single atoms catalysts with high catalytic activity and stability for advanced green energy conversion technologies.

Failure Mechanism, Electrolyte Design, and Electrolyte/Electrode Interface Regulation for Low-Temperature Zinc-Based Batteries.

With more renewable energy developed to satisfy the human need in the energy crisis, electricity storage is critical in power utilization and storage. Due to its high safety, high nature reserve, and high energy density, the zinc-based battery is drawing increasing attention. Together with the expansion of human activities, the low-temperature battery is developed to satisfy the power demand in extreme environments, and as a critical component, electrolytes shall have a low freezing point and satisfying electrochemical properties in cold conditions. In this review, the development of low-temperature electrolytes for zinc-based batteries will be comprehensively introduced. First, the failure mechanism of zinc-based battery at low temperature will be illustrated. Second, five main types of low-temperature electrolytes will be introduced in detail. Finally, the regulation of electrolyte/electrode surface at low temperature will be discussed. This review aims to provide a guideline for low-temperature electrolyte design from the perspective of molecular behavior regulation.