Abstract:In recent years, the development of aqueous lithium‐ion batteries and aqueous zinc‐ion batteries has received extensive attention thanks to the advantages of high safety, environmental friendliness, and easy assembly conditions. However, aqueous batteries are always restricted in terms of limited cycling stability and low energy density due to their intrinsically narrow electrochemical window, hydrogen evolution, and side reactions. These problems can be remarkably alleviated by hybridizing aqueous/non‐aqueous… Show more
Aqueous batteries are attractive due to their high safety and fast reaction kinetics, but the narrow electrochemical stability window of H2O limits their applications. It is a big challenge to broaden the electrochemical operation window of aqueous electrolytes while retaining fast reaction kinetics. Here, a new organic aqueous mixture electrolyte of manipulatable (3D) molecular microheterogeneity with H2O‐rich and H2O‐poor domains is demonstrated. H2O‐poor domains molecularly surround the reformed microclusters of H2O molecules through interfacial H‐bonds, which thus not only inhibit the long‐range transfer of H2O but also allow fast and consecutive Li+ transport. This new design enables low‐voltage anodes reversibly cycling with aqueous‐based electrolytes and high ionic conductivity of 4.5 mS cm−1. LiMn2O4||Li4Ti5O12 full cells demonstrate excellent cycling stability over 1000 cycles under various C rates and a low temperature of −20 °C. 1 Ah pouch cell delivers a high energy density of 79.3 Wh kg−1 and high Coulombic efficiency of 99.4% at 1 C over 200 cycles. This work provides new insights into the design of electrolytes based on the molecular microheterogeneity for rechargeable batteries.
Aqueous batteries are attractive due to their high safety and fast reaction kinetics, but the narrow electrochemical stability window of H2O limits their applications. It is a big challenge to broaden the electrochemical operation window of aqueous electrolytes while retaining fast reaction kinetics. Here, a new organic aqueous mixture electrolyte of manipulatable (3D) molecular microheterogeneity with H2O‐rich and H2O‐poor domains is demonstrated. H2O‐poor domains molecularly surround the reformed microclusters of H2O molecules through interfacial H‐bonds, which thus not only inhibit the long‐range transfer of H2O but also allow fast and consecutive Li+ transport. This new design enables low‐voltage anodes reversibly cycling with aqueous‐based electrolytes and high ionic conductivity of 4.5 mS cm−1. LiMn2O4||Li4Ti5O12 full cells demonstrate excellent cycling stability over 1000 cycles under various C rates and a low temperature of −20 °C. 1 Ah pouch cell delivers a high energy density of 79.3 Wh kg−1 and high Coulombic efficiency of 99.4% at 1 C over 200 cycles. This work provides new insights into the design of electrolytes based on the molecular microheterogeneity for rechargeable batteries.
Electrolytes play a crucial role in facilitating the ionic movement between cathode and anode, which is essential for the flow of electric current during the charging and discharging process of the rechargeable batteries. In particular, electrolyte additives are considered as effective and economical approaches into the advancements of the battery technologies in both the conventional non‐aqueous and burgeoning aqueous electrolyte systems. Herein, a systematic and comprehensive review of the electrolyte additives is reported for the interfacial engineering of Li and Zn metal anodes in the non‐aqueous and aqueous electrolytes, respectively. The types of electrolyte additives and their corresponding functionalities for the protection of these two metal anodes are discussed along with the electrochemical features of solid electrolyte interphase (SEI) derived from electrolyte additives. The recent progress on electrolyte additives for these two battery systems are also addressed from the perspectives of electrode, electrolyte, and the associated SEI. Finally, the outlook and perspective on the current issues and future directions in the field of electrolyte additive engineering are presented for next‐generation battery technologies beyond the conventional Li‐ion batteries.
Herein, a facile hydrothermal method is utilized to prepare a (NH4)2V7O16/reduced graphene oxide (rGO) composite. In an aqueous electrolyte, the obtained (NH4)2V7O16/rGO exhibits superior lithium storage characteristics compared to pure (NH4)2V7O16 in both the three‐electrode configuration and full cell. This improvement can be ascribed to the synergistic effects of incorporation of defective oxygen and rGO modification. The present study proposes a feasible strategy for enhancing the electrochemical properties of (NH4)2V7O16 and demonstrates the potential of the (NH4)2V7O16/rGO composite for aqueous rechargeable lithium‐ion batteries.
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