Pathways Toward High-energy Li-sulfur Batteries, Identified via Multi-reaction Chemical Modeling
Pathways Toward High-energy Li-sulfur Batteries, Identified via Multi-reaction Chemical Modeling
复制标题
通过多反应化学模型确定高能锂硫电池的途径
DOI：
10.1149/1945-7111/ac4541
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发表时间：
2022
影响因子：
3.9
通讯作者：
DeCaluwe, Steven C.
中科院分区：
文献类型：
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作者：
Korff, Daniel;Colclasure, Andrew M.;Ha, Yeyoung;Smith, Kandler A.;DeCaluwe, Steven C.
在这里，我们提出了一个一维模型的锂硫电池的物理推导的几何参数和化学一致的电化学动力学。该方法可以直接比较所提出的Li-S机制，并深入了解多硫化物中间体对电池放电的影响。比较多种机制的预测表明，锂化和非锂化多硫化物物种的需要，并强调了复杂的电化学机制的参数估计开发的挑战。该模型也被用来探索阴极设计策略。电解质/硫比在2-4 μL mg− 1范围内的放电性能和多硫化物浓度确定了限制电池能量和功率密度的权衡，并强调了多硫化物沉淀的风险。新的阴极和电解质方法必须限制电解质中的多硫化物浓度，以释放Li-S技术中更好的倍率性能，并防止由于多硫化物沉淀而导致的容量衰减。
Here we present a 1D model of a Li-Sulfur battery with physically derived geometric parameters and thermodynamically consistent electrochemical kinetics. The approach enables straightforward comparison of proposed Li-S mechanisms and provides insights into the influence of polysulfide intermediates on battery discharge. Comparing predictions from multiple mechanisms demonstrates the need for both lithiated and non-lithiated polysulfide species, and highlights the challenge of developing parameter estimates for complex electrochemical mechanisms. The model is also used to explore cathode design strategies. Discharge performance and polysulfide concentrations for electrolyte/sulfur ratios in the range 2–4 μL mg− 1 identifies trade-offs that limit battery energy and power density, and highlights the risk of polysulfide precipitation. New cathode and electrolyte approaches must limit polysulfide concentrations in the electrolyte, both to unlock better rate capabilities in Li-S technology and to prevent capacity fade due to polysulfide precipitation.