Ultra-High Fluorine Enhanced Homogeneous Nucleation of Lithium Metal on Stepped Carbon Nanosheets with Abundant Edge Sites

Xiao Jian; Xiao Nan; Li KaiZhang LipengChang JiangweiMa XiaoqingLi HongqiangBai JinpengJiang QikeQiu Jieshan

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Ultra-High Fluorine Enhanced Homogeneous Nucleation of Lithium Metal on Stepped Carbon Nanosheets with Abundant Edge Sites

机译：Ultra-High Fluorine Enhanced Homogeneous Nucleation of Lithium Metal on Stepped Carbon Nanosheets with Abundant Edge Sites

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Disordered nucleation sites and a fragile solid electrolyte interphase on the reactive interface tend to cause uncontrolled growth of lithium dendrites, which induce severe safety concerns and prevent lithium metal batteries from finding practical applications. Herein, novel stepped carbon nanosheets with abundant step edges and ultra-high fluorine content (37.44 at%) are fabricated by combining an improved molten salt synthesis method with C4F8 vacuum plasma treatment. The solvent-induced spatial confinement effect, i.e., orientation carbonization of pitch macromolecules, leads to the formation of step-edge-enriched nanoarrays. Meanwhile, the adequate exposure of edge sites on the basal plane of carbon nanosheets is conducive to achieve the ultra-efficient doping of elemental fluorine in only 10 min. Further experiments and theoretical calculations demonstrate that the coupling effect of sufficient edge sites and active semi-ionic C-F/covalent CF2 groups on the carbon surface can not only form 2D fluorinated lithium chain and a robust Li-F network, but also effectively facilitate Li ion redox kinetics and morphological stability, presenting a step-edge-guided plating process. As such, the developed anodes deliver an ultra-low nucleation overpotential (approximate to 10.5 mV), high Coulombic efficiency (98% over 385 cycles), ultra-long cycling duration for up to 3000 h under approximate to 10 mV, and excellent full battery performance.

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《Advanced energy materials》 |2022年第10期|2103123.1-2103123.14|共14页
作者
Xiao Jian; Xiao Nan; Li KaiZhang LipengChang JiangweiMa XiaoqingLi HongqiangBai JinpengJiang QikeQiu Jieshan;
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作者单位

Dalian Univ Technol, State Key Lab Fine Chem, Sch Chem Engn, Liaoning Key Lab Energy Mat & Chem Engn, Dalian 116024, Liaoning, Peoples R China;

Beijing Univ Chem Technol, Coll Chem Engn, State Key Lab Organ Inorgan Composites, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China;

Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116024, Liaoning, Peoples R ChinaDalian Univ Technol, State Key Lab Fine Chem, Sch Chem Engn, Liaoning Key Lab Energy Mat & Chem Engn, Dalian 116024, Liaoning, Peoples R China|Beijing Univ Chem Technol, Coll Chem Engn, State Key Lab Organ Inorgan Composites, Beijing Adv Innovat Ctr Soft;

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LiF; lithium anodes; step-edge-guided nucleation; stepped carbon nanosheets; fluorine;

Ultra-High Fluorine Enhanced Homogeneous Nucleation of Lithium Metal on Stepped Carbon Nanosheets with Abundant Edge Sites

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