Carbonate electrolytes have excellent chemical stability and high salt solubility, which is ideally practical choice for achieving high energy density sodium (Na) metal battery at room temperature. However, their application at ultra-low temperature (-40 oC) is adversely affected by the instability of solid electrolyte interphase (SEI) formed by electrolyte decomposition and the difficulty of desolvation. Here, we designed a novel low-temperature carbonate electrolyte by molecular engineering on solvation structure. The calculations show that ethylene sulfate (ES) inhibits solvent decomposition and reduces the sodium ion desolvation energy. In addition, experimental results demonstrate that ES promotes the forming of more inorganic substances on the Na surface, which inhibits dendrite growth and increases ionic conductivity. At -40 oC, the Na||Na symmetric battery exhibits a stable cycle of 1500 hours, and the Na||Na3V2(PO4)3 (NVP) battery achieves 88.2% capacity retention after 200 cycles. Our work provides a new way to develop high energy density sodium metal battery under extreme low temperature environment.

Molecular Engineering on Solvation Structure of Carbonate Electrolyte toward Durable Sodium Metal Battery at -40 oC.

Constructing an inorganic-rich and robust solid electrolyte interphase (SEI) is one of the crucial approaches to improving the electrochemical performance of sodium metal batteries (SMBs). However, the low conductivity and distribution of common inorganics in SEI disturb Na+ diffusion and induce nonuniform sodium deposition. Here, we construct a unique SEI with evenly scattered high-conductivity inorganics by introducing a self-sacrifice LiTFSI into the sodium salt-base carbonate electrolyte. The reductive competition effect between LiTFSI and FEC facilitates the formation of the SEI with evenly scattered inorganics. In which the high-conductive Li3N and inorganics provide fast ions transport domains and high-flux nucleation sites for Na+, thus conducive to rapid sodium deposition at a high rate. Therefore, the SEI derived from LiTFSI and FEC enables the Na∥Na3V2(PO4)3 cell to show 89.15% capacity retention (87.62 mA h g-1) at an ultrahigh rate of 60 C after 10,000 cycles, while the cell without LiTFSI delivers only 48.44% capacity retention even after 8000 cycles. Moreover, the Na∥Na3V2(PO4)3 pouch cell with the special SEI presents a stable capacity retention of 92.05% at 10 C after 2000 cycles. This unique SEI design elucidates a new strategy to propel SMBs to operate under extreme high-rate conditions.

Reductive Competition Effect-Derived Solid Electrolyte Interphase with Evenly Scattered Inorganics Enabling Ultrahigh Rate and Long-Life Span Sodium Metal Batteries.

The sodium (Na)‐metal anode with high theoretical capacity and low cost is promising for construction of high‐energy‐density metal batteries. However, the unsatisfactory interface between Na and the liquid electrolyte induces tardy ion transfer kinetics and dendritic Na growth, especially at ultralow temperature (−40 °C). Herein, an artificial heterogeneous interphase consisting of disodium selenide (Na2Se) and metal vanadium (V) is produced on the surface of Na (Na@Na2Se/V) via an in situ spontaneous chemical reaction. Such interphase layer possesses high sodiophilicity, excellent ionic conductivity, and high Young's modulus, which can promote Na‐ion adsorption and transport, realizing homogenous Na deposition without dendrites. The symmetric Na@Na2Se/V cell exhibits outstanding cycling life span of over 1790 h (0.5 mA cm−2/1 mAh cm−2) in carbonate‐based electrolyte. More remarkably, ab initio molecular dynamics simulations reveal that the artificial Na2Se/V hybrid interphase can accelerate the desolvation of solvated Na+ at −40 °C. The Na@Na2Se/V electrode thus exhibits exceptional electrochemical performance in symmetric cell (over 1500 h at 0.5 mA cm−2/0.5 mAh cm−2) and full cell (over 700 cycles at 0.5 C) at −40 °C. This work provides an avenue to design artificial heterogeneous interphase layers for superior high‐energy‐density metal batteries at ambient and ultralow temperatures.

A Multifunctional Interphase Layer Enabling Superior Sodium‐Metal Batteries under Ambient Temperature and −40 °C

Lithium batteries play a dominant role in the power source market of electric vehicles and portable electronic devices. The electrolyte is critical to determining the performance of lithium batteries. Conventional electrolytes cannot meet the ever-growing demands of fast-charging, wide-temperature operation, and safety properties of lithium batteries. Despite the great success of (localized) high-concentration electrolytes, they still suffer from disadvantages like low ionic conductivity and high cost. The emerging weakly solvating electrolytes, also known as low-solvating electrolytes, offer another solution to these challenges and have attracted intensive research interests in recent years. This contribution reviews the working mechanisms, design principles, and recent advances in developing weakly solvating electrolytes. A summary and perspective about future research directions in this field is also provided. The insights will benefit both academic and industrial communities in designing safe and high-performance next-generation Li batteries. 

Weakly solvating electrolytes for next-generation lithium batteries: design principles and recent advances

Sodium‐ion batteries (SIBs), driven by sustainability and cost advantage, have been recognized as one of the most promising electrochemical energy storage devices. Electrolytes, as the most unique component that not only ionically connect while insulating electronically electrodes but also determine the eventual improvements in performance mainly regarding cycle life, Coulombic efficiency, energy density, and safety, hold the key to the practical implementation of SIBs. In this review, the fundamental design principles of Na+‐ion electrolytes and the chemical properties of the Na+ cation over the Li+ cation in terms of ion transport, salt dissolution, and solvation structure are first discussed. Then, a sequence of crucial experimental discoveries and strategical achievements in the field of electrolytes for SIBs are presented, with focuses on the ether‐based electrolytes for co‐intercalation into graphite, diluted and highly concentrated electrolytes, wide temperature range electrolytes, nonflammable electrolytes, indispensable electrolyte components (functional additives and new sodium salts). Finally, a detailed analysis of research trends of practically feasible Na+‐ion electrolytes is presented to aid in the ongoing quest for better SIBs of the future.

Nonaqueous Liquid Electrolytes for Sodium‐Ion Batteries: Fundamentals, Progress and Perspectives

Low-temperature and high-rate sodium metal batteries enabled by electrolyte chemistry

The possibility of utilizing quantum effects to enhance the performance of quantum heat engines has been an active topic of research, but how to enhance the performance by optimizing the engine parameters needs to be further studied. In this study, the temperature difference and dissipation modes affecting the performance of a three-level quantum heat engine were analyzed using an orthogonal test. The results indicated that the dissipation mode dominated the performance of the quantum heat engine. The quantum heat engine performs best when there is only resonance and no detuning; however, when detuning exists, a lower resonance can improve the efficiency by reducing energy losses. Regarding the temperature difference, the best performance was achieved at a medium temperature difference owing to the decreasing heat leakage. Finally, the “quantum friction” caused by the detuning could make the maximal efficiency lower than the Carnot efficiency.

https://aip.scitation.org/doi/pdf/10.1063/5.0139998

Continuous three-level quantum heat engine with high performance under medium temperature difference

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Low-temperature and high-rate sodium metal batteries enabled by electrolyte chemistry

Continuous three-level quantum heat engine with high performance under medium temperature difference