High‐Performance Organic Lithium Batteries with an Ether‐Based Electrolyte and 9,10‐Anthraquinone (AQ)/CMK‐3 Cathode

Abstract

Organic carbonyl electrode materials of lithium batteries have shown multifunctional molecule design and high capacity, but have the problems of poor cycling and low rate performance due to their high solubility in traditional carbonate‐based electrolytes and low conductivity. High‐performance organic lithium batteries with modified ether‐based electrolyte (2 m LiN(CF3SO2)2 in 1,3‐dioxolane/dimethoxyethane solvent with 1% LiNO3 additive (2m‐DD‐1%L)) and 9,10‐anthraquinone (AQ)/CMK‐3 (AQC) nanocomposite cathode are reported here. The electrochemical results manifest that 2m‐DD‐1%L electrolyte promotes the cycling performance due to the restraint of AQ dissolution in ether‐based electrolyte with high Li salt concentration and formation of a protection film on the surface of the anode. Additionally, the AQC nanocomposite improves the rate performance because of the nanoconfinement effect of CMK‐3 and the decrease of charge transfer impedance. In 2m‐DD‐1%L electrolyte, AQC nanocomposite delivers an initial discharge capacity of 205 mA h g−1 and a capacity of 174 mA h g−1 after 100 cycles at 0.2 C. Even at a high rate of 2 C, its capacity is 146 mA h g−1. This strategy is also used for other organic carbonyl compounds with quinone substructures and they maintain high stable capacities. This sheds light on the development of advanced organic lithium batteries with carbonyl electrode materials and ether‐based electrolytes.

Molecular Engineering with Organic Carbonyl Electrode Materials for Advanced Stationary and Redox Flow Rechargeable Batteries

“…For example, adopting electrolyte additives, such as LiNO 3 [51] and FEC, [118] to form a solid electrolyte interface (SEI) film on the anode or cathode is beneficial for the stabilization of the electrode. In addition, the easily dissolved carbonyls (raw materials or radical products) are shuttled to the Li anode with side reactions, resulting in low Coulombic efficiency and poor cycling stability.…”

“…Ingenious strategies of molecular engineering, [36,37] nanosizing, [38,39] fabricating hybrid materials, [40][41][42][43][44][45][46][47][48] and electrolyte optimization [49][50][51][52][53][54] have been adopted to overcome their intrinsic drawbacks (e.g., high solvency and poor conductivity). Ingenious strategies of molecular engineering, [36,37] nanosizing, [38,39] fabricating hybrid materials, [40][41][42][43][44][45][46][47][48] and electrolyte optimization [49][50][51][52][53][54] have been adopted to overcome their intrinsic drawbacks (e.g., high solvency and poor conductivity).…”

Anthraquinone‐Based Oligomer as a Long Cycle‐Life Organic Electrode Material for Use in Rechargeable Batteries

“…9,10-Anthraquinone (AQ) (Figure 1a) is an example which shows a high utilization ratio during the first discharge process; [8] however, the electrode using AQ itself significantly deteriorates during cycling. While the applications of some special binder, [21] separator, [22] and electrolyte solutions [23] containing additives have been recently reported to have a positive effect for this issue; however, the development of a long cycle-life active material itself based on a new molecular design would be important at the same time. [18][19][20] To improve the cycling stability, suppressing the dissolution should be inevitable.…”

Advancing Electrolytes Towards Stable Organic Batteries

“…In a study on AQ in LiTFSI-dioxolane/DME electrolytes, Zhang et al found that a middling concentration (2 M) gave the highest cycling stability. [27] The concentration of the electrolyte also influenced the voltage profile of AQ: while a single plateau was observed in 1 and 2 M electrolytes, further increase to 3 and 4 M split the plateau into two. Although the dissolution of AQ was not fully suppressed in these electrolytes, stable cycling can still be achieved by using a LiNO3 additive which formed a protective layer on the surface of the lithium anode and prevented reaction between AQ and lithium.…”