共轭微孔聚合物微球的气相氟化可有效稳定锂金属阳极的界面,Carbon Energy

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共轭微孔聚合物微球的气相氟化可有效稳定锂金属阳极的界面
Carbon Energy ( IF 19.5 ) Pub Date : 2023-03-10 , DOI: 10.1002/cey2.354
Zihao Li ₁ , Lingchen Kong ₁ , Cong Peng ₁ , Wei Feng _{1,

2}

Affiliation

锂（Li）金属负极因其超高的理论容量和低电势而受到广泛关注。然而，不稳定的电极/电解质界面附近锂的不均匀沉积导致锂枝晶的生长和活性电极的退化。在此，我们用氟气（F ₂）直接氟化含炔的共轭微孔聚合物（ACMP）微球，引入一种新型氟化中间层作为锂金属电池的界面稳定剂。利用密度泛函理论方法，发现所制备的氟化ACMP（FACMP）具有丰富的部分离子C-F键。具有电化学不稳定性的C-F键在循环过程中产生显着的亲锂性。活性C-F键和锂离子之间的原位反应使氟化锂微晶转移到固体电解质中间相（SEI）层，保证有效的离子分布和顺利的锂沉积。因此，具有氟化中间层的锂金属电极在使用双（三氟甲磺酰基）亚胺锂电解质以及非氟化双（草酸）硼酸锂电解质体系的半电池和全电池中表现出优异的循环性能。该策略对于可定制的 SEI 层非常重要，可稳定电极界面并确保锂金属阳极的高利用率，特别是在非氟化电解质中。

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Gas-phase fluorination of conjugated microporous polymer microspheres for effective interfacial stabilization in lithium metal anodes

Lithium (Li) metal anodes have attracted extensive attention due to their ultrahigh theoretical capacity and low potential. However, the uneven deposition of Li near the unstable electrode/electrolyte interfaces leads to the growth of Li dendrites and the degradation of active electrodes. Herein, we directly fluorinate alkyne-containing conjugated microporous polymers (ACMPs) microspheres with fluorine gas (F₂) to introduce a novel fluorinated interlayer as an interfacial stabilizer in lithium metal batteries. Using density functional theory methods, it is found that as-prepared fluorinated ACMP (FACMP) has abundant partially ionic C–F bonds. The C–F bonds with electrochemical lability yield remarkable lithiophilicity during cycling. The in situ reactions between the active C–F bonds and Li ions enable transfer of lithium fluoride microcrystals to the solid electrolyte interphase (SEI) layers, guaranteeing effective ionic distribution and smooth Li deposition. Consequently, Li metal electrodes with the fluorinated interlayers demonstrate excellent cycling performances in both half-batteries and full cells with a lithium bis(trifluoromethanesulfonyl)imide electrolyte as well as a nonfluorinated lithium bis(oxalate)borate electrolyte system. This strategy is highly significant in customizable SEI layers to stabilize electrode interfaces and ensure high utilization of Li metal anodes, especially in a nonfluorinated electrolyte.

更新日期：2023-03-10

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