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Anchoring Lithium Polysulfides via Affinitive Interactions: Electrostatic Attraction, Hydrogen Bonding, or in Parallel?
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2015-08-24 00:00:00 , DOI: 10.1021/acs.jpcc.5b06373
Zhuan Ji 1 , Bo Han 1 , Qiyang Li 1 , Chenggang Zhou 1 , Qiang Gao 1 , Kaisheng Xia 1 , Jinping Wu 1
Affiliation  

Stabilizing lithium polysulfides in cathodes via interactions between polysulfides and affinitive functional groups could prevent polysulfide dissolution, leading to suppressed “shuttle effect” of lithium/sulfur (Li/S) batteries. Herein, four deoxynucleotides (DNs), including A (adenine-DN), T (thymine-DN), G (guanine-DN), and C (cytosine-DN), which own rich polysulfide affinitive groups, are selected to model the anchoring environments of polysulfides. Using the most soluble Li2S8 as probe, our first-principles simulations suggest that the interactions between polysulfides and substrates are highly correlated to the charges of affinitive sites, H-bonding environments and structural tension. The contributions from each type of interactions are quasi-quantitatively assessed. The electrostatic attractions between Li+ and the strong electron lone-pairs dominate the adsorption energetics, while the H-bonds formed between S82– and substrate give rise to excessive stabilization. In contrast, structural distortion or rearrangement of the substrates is detrimental to the anchoring strengths. The quasi-quantitative resolution on the different interaction modes provides a facile and rational scheme for screening more efficient polysufide affinitive additives to sustain the cathode cyclicity of Li/S batteries.

中文翻译:

通过亲和相互作用固定多硫化锂:静电吸引,氢键结合或平行反应?

通过多硫化物与亲和性官能团之间的相互作用稳定阴极中的多硫化锂可以防止多硫化物溶解,从而抑制锂/硫(Li / S)电池的“穿梭效应”。在此,选择四个具有丰富的多硫亲和基团的脱氧核苷酸(DN),包括A(腺嘌呤-DN),T(胸腺嘧啶-DN),G(鸟嘌呤-DN)和C(胞嘧啶-DN)。多硫化物的锚固环境。使用最易溶的Li 2 S 8作为探针,我们的第一性原理模拟表明多硫化物与底物之间的相互作用与亲和力,H键环境和结构张力高度相关。每种类型的相互作用的贡献都进行了定量评估。Li +和强电子孤对之间的静电吸引力主导着吸附能,而S 8 2–之间形成的H键和底物会引起过度的稳定性。相反,基板的结构变形或重新布置不利于锚固强度。不同相互作用模式下的准定量分辨率为筛选更有效的聚硫亲和添加剂以维持Li / S电池的阴极循环性提供了一种简便合理的方案。
更新日期:2015-08-24
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