Anthraquinone-Based Silicate Covalent Organic Frameworks as Solid Electrolyte Interphase for High-Performance Lithium–Metal Batteries

• DOI: 10.1021/jacs.3c06723
• Publication Date: 2023-11-02T11:14:36Z
• Authors: Chen Li; Dan-Dong Wang; Gerald Siu Hang P...; Zhengyang Zhang; Jun Huang; Ki-Taek Bang; Chun Yin Lau; Shao-Yuan Leu; Yanming Wang; Yoonseob Kim
• Keywords: Anthraquinones

Lithium (Li)-metal batteries (LMBs) possess the highest theoretical energy density among current battery designs and thus have enormous potential for use in storage. However, development of LMBs has been severely hindered by safety concerns arising from dendrite growth unstable interphases on Li anode. Covalent organic frameworks (COFs) incorporating either redox-active or anionic moieties their backbones high Li-ion (Li+) conductivities mechanical/chemical stabilities, so are promising solid electrolyte (SEIs) LMBs. Here, we synthesized anthraquinone-based silicate COFs (AQ-Si-COFs) that contained both sites via condensation tetrahydroxyanthraquinone with silicon dioxide. The nine Li+-mediated charge/discharge processes enabled AQ-Si-COF to demonstrate an ionic conductivity 9.8 mS cm-1 at room temperature a single-ion-conductive transference number 0.92. Computational studies also supported Li+ mechanism. We used as interphase LMB cells LiCoO2 cathode attained maximum reversible capacity 188 mAh g-1 0.25 C during high-voltage operation. Moreover, this cell demonstrated suppressed stable cyclability, its decreasing less than 3% up 100 cycles. These findings effectiveness our practical utility SEI LMB.