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利用固相合成的硼掺杂碳点调控锂负极的有序沉积

倪佳文,黄遵辉,宋天兵,马千里,何天乐,张熙荣,熊焕明   

  1. 复旦大学化学系,上海市分子催化和功能材料重点实验室,上海 200438
  • 收稿日期:2024-04-12 修回日期:2024-05-03 出版日期:2024-05-08 发布日期:2024-05-08
  • 通讯作者: 熊焕明 E-mail:hmxiong@fudan.edu.cn
  • 基金资助:
    国家自然科学基金(批准号:21975048)和上海市自然科学基金(批准号:19DZ2270100)资助.

Ordered Lithium Deposition on Lithium Metal Anode Controlled by Boron-Doped Carbon Dots Produced from Solid-State Synthesis

NI Jiawen, HUANG Zunhui, SONG Tianbing, MA Qianli, HE Tianle, ZHANG Xirong, XIONG Huanming   

  1. Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, China
  • Received:2024-04-12 Revised:2024-05-03 Online:2024-05-08 Published:2024-05-08
  • Contact: XIONG Huanming E-mail:hmxiong@fudan.edu.cn
  • Supported by:
    Supported by the National Natural Science Foundation of China(No.21975048) and the Shanghai Science and Technology Committee, China(No.19DZ2270100).

摘要: 通过固相合成制备了一种硼掺杂的碳点并将其作为锂电池的电解液添加剂。在空气中催化热解碳源制备碳点,产量大、产率高、安全可控、操作方便。以间苯三酚和硼酸为原料合成的硼掺杂碳点,在碳酸酯类电解液中具有良好的分散性。掺杂的硼原子作为缺电子中心,可以通过路易斯酸碱作用结合含氟阴离子基团,从而诱导锂离子均匀沉积到锂金属负极上。当这种碳点的添加量为0.3 mg mL-?1时,锂对称电池在电流为0.5 mA cm-2,电沉积量为0.5 mAh cm-2的测试条件下可稳定循环2500 h,说明该碳点添加剂极大地提升了锂沉积/溶解的可逆性。使用碳点添加后的电解液组装磷酸铁锂全电池,初始容量144.4 mAh g-1,100次循环后容量保留率可以达到95.1%。本工作展示了硼掺杂的碳点在提高锂电池工作性能方面独特的优势。

关键词: 碳点, 硼掺杂, 电化学储能, 电解质添加剂, 锂金属负极

Abstract: Boron-doped carbon dots (B-CDs) synthesized via solid-phase method were employed as electrolyte additives for lithium metal batteries. The carbon dots were prepared through the catalytic pyrolysis of carbon sources in air, highlighting high yield, efficiency, safety, and convenience. Synthesized from 1,3,5-trihydroxy-benzen and boric acid, the B-CDs exhibited excellent dispersibility in carbonate-based electrolytes. The doped boron atoms, serving as electron-deficient centers, could engage fluorinated anion groups through Lewis acid-base interactions, thus inducing uniform lithium-ion deposition on the lithium anode. At an additive concentration of 0.3 mg mL-1, a lithium symmetric cell demonstrated stable cycling for 2500 hours under a current density of 0.5 mA cm-2 and a plating capacity of 0.5 mAh cm-2, indicating that the carbon dot additive significantly enhanced the reversibility of lithium deposition/dissolution. When these carbon dots were incorporated into electrolytes of a LiFePO4 full cell, an initial capacity of 144.4 mAh g-1 was achieved, with a capacity retention of 95.1% after 100 cycles. This work showcases the unique advantages of boron-doped carbon dots in improving the operational performance of lithium metal batteries.

Key words: Carbon dots, Boron doping, Electrochemical energy storage, Electrolyte additives, Lithium metal anode

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