The serious dissolution of organic electrode materials (e.g., perylene-3,4,9,10-tetracarboxylic dianhydride, PTCDA) in electrolytes is a major challenge, deteriorating their electrochemical performances and hindering the interpretation of the fundamental redox reaction mechanisms including the intrinsic kinetics and the solvent cointercalation. To address these issues, we propose a rationally designed sulfonamide-based electrolyte to enable a quasi-solid-state conversion (QSSC) of the PTCDA cathode by effectively suppressing its dissolution in the electrolyte. Benefiting from the QSSC, the Li||PTCDA cells can retain ∼95.8% of the original capacity after 300 cycles with both high and stable energy efficiencies >95%, even comparable to the layered transition-metal oxide cathodes, greatly outperforming an ether-based electrolyte with a high PTCDA solubility. The high energy efficiencies indicate that the QSSC of PTCDA has intrinsic fast redox kinetics. Furthermore, the solvent cointercalation mechanism was investigated by density functional theory/molecular dynamic calculations. This work develops a strategy for designing electrolytes for highly stable and efficient Li–organic batteries.

中文翻译：

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在锂有机电池中，由磺胺基电解质实现具有快速氧化还原动力学的准固态转换


有机电极材料（例如，苝-3,4,9,10-四羧酸二酐，PTCDA）在电解质中的严重溶解是一项重大挑战，会恶化其电化学性能并阻碍对基本氧化还原反应机理的解释，包括本征动力学和溶剂共插层。为了解决这些问题，我们提出了一种合理设计的磺胺基电解质，通过有效抑制 PTCDA 阴极在电解质中的溶解来实现其准固态转换 （QSSC）。受益于 QSSC，Li||PTCDA 电池在 300 次循环后仍能保持 ∼95.8% 的原始容量，具有高且稳定的能效 >95%，甚至可以与层状过渡金属氧化物阴极相媲美，大大优于具有高 PTCDA 溶解度的醚基电解质。高能量效率表明 PTCDA 的 QSSC 具有固有的快速氧化还原动力学。此外，通过密度泛函理论/分子动力学计算研究了溶剂共插层机制。这项工作开发了一种为高度稳定和高效的锂-有机电池设计电解质的策略。