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Aqueous Li-ion battery enabled by halogen conversion-intercalation chemistry in graphite

机译：通过石墨中的卤素转化嵌入化学使水性锂离子电池

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摘要

The use of 'water-in-salt' electrolytes has considerably expanded the electrochemical window of aqueous lithium-ion batteries to 3 to 4 volts, making it possible to couple high-voltage cathodes with low-potential graphite anodes(1-4). However, the limited lithium intercalation capacities (less than 200 milliampere-hours per gram) of typical transition-metal-oxide cathodes(5,6) preclude higher energy densities. Partial(7,8) or exclusive(9) anionic redox reactions may achieve higher capacity, but at the expense of reversibility. Here we report a halogen conversion-intercalation chemistry in graphite that produces composite electrodes with a capacity of 243 milliampere-hours per gram (for the total weight of the electrode) at an average potential of 4.2 volts versus Li/Li+. Experimental characterization and modelling attribute this high specific capacity to a densely packed stage-I graphite intercalation compound, C-3.5[Br0.5Cl0.5], which can form reversibly in water-in-bisalt electrolyte. By coupling this cathode with a passivated graphite anode, we create a 4-volt-class aqueous Li-ion full cell with an energy density of 460 watt-hours per kilogram of total composite electrode and about 100 per cent Coulombic efficiency. This anion conversion-intercalation mechanism combines the high energy densities of the conversion reactions, the excellent reversibility of the intercalation mechanism and the improved safety of aqueous batteries.
机译：使用“盐水”电解质的用途可显着扩展到3至4伏的水锂离子电池的电化学窗口，使得可以将具有低电位石墨阳极（1-4）的高压阴极耦合。然而，典型的过渡金属氧化物阴极（5,6）的有限锂插入容量（每克/克/克的每克）排除了更高的能量密度。部分（7,8）或独家（9）阴离子氧化还原反应可能达到更高的容量，但以牺牲可逆性为代价。在这里，我们在石墨中报道了一种卤素转化 - 插层化学，其在4.2伏与Li / Li +的平均电位下产生每克243毫安 - 小时（电极总重量）的复合电极。实验表征和建模将这种高特定容量归因于密集包装的阶段-I石墨嵌入化合物，C-3.5 [BR0.5CL0.5]，其可以在水 - 抗体电解质中可逆地形成。通过将该阴极与钝化的石墨阳极耦合，我们通过每千克/千克总复合电极的能量密度为460瓦特小时的能量密度和约100％的库仑效率，通过耦合4伏级锂离子全电池。这种阴离子转化晶体化机制结合了转化反应的高能量密度，嵌入机理的优异可逆性以及含水电池的改善安全性。

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  • 来源
    《Nature》 |2019年第7755期|245-250|共6页
  • 作者

    Yang Chongyin; Chen Ji; Ji Xiao; Pollard Travis P.; Lu Xujie; Sun Cheng-Jun; Hou Singyuk; Liu Qi; Liu Cunming; Qing Tingting; Wang Yingqi; Borodin Oleg; Ren Yang; Xu Kang; Wang Chunsheng;

  • 作者单位

    Univ Maryland Dept Chem & Biomol Engn College Pk MD 20742 USA;

    Univ Maryland Dept Chem & Biomol Engn College Pk MD 20742 USA;

    Univ Maryland Dept Chem & Biomol Engn College Pk MD 20742 USA;

    US Army Electrochem Branch Power & Energy Div Sensor & Electron Devices Directorate Res Lab Adelphi MD USA;

    Ctr High Pressure Sci & Technol Adv Res Shanghai Peoples R China;

    Argonne Natl Lab Adv Photon Source Xray Sci Div Argonne IL 60439 USA;

    Univ Maryland Dept Chem & Biomol Engn College Pk MD 20742 USA;

    Argonne Natl Lab Adv Photon Source Xray Sci Div Argonne IL 60439 USA|City Univ Hong Kong Dept Phys Hong Kong Peoples R China;

    Argonne Natl Lab Adv Photon Source Xray Sci Div Argonne IL 60439 USA;

    Univ Maryland Dept Chem & Biomol Engn College Pk MD 20742 USA;

    Ctr High Pressure Sci & Technol Adv Res Shanghai Peoples R China;

    US Army Electrochem Branch Power & Energy Div Sensor & Electron Devices Directorate Res Lab Adelphi MD USA;

    Argonne Natl Lab Adv Photon Source Xray Sci Div Argonne IL 60439 USA;

    US Army Electrochem Branch Power & Energy Div Sensor & Electron Devices Directorate Res Lab Adelphi MD USA;

    Univ Maryland Dept Chem & Biomol Engn College Pk MD 20742 USA|Univ Maryland Dept Chem & Biochem College Pk MD 20742 USA;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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