Emma Kaeli, Zhelong Jiang, Xiaomian Yang, Emma P. K. L. Choy, Nicolas B. Liang, Edward Barks, Sunny Wang, Stephen Dongmin Kang and William C. Chueh
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引用次数: 0
摘要
固态电池(SSBs)比液态电解质锂离子电池(lib)具有更高的能量密度。然而,由于界面反应,ssb的第一周期容量损失高于lib。SSBs中关键界面的化学演化已被广泛表征。然而,电化学上,我们缺乏一种通用的策略来量化固体电解质(SE)氧化还原的可逆性,用于已建立的和下一代SSB电解质。在这项工作中,我们通过定制的电化学测试和operando x射线衍射来解开由Li6PS5Cl SE, Li(Ni0.5Mn0.3Co0.2)O2 (NMC)和碳导电添加剂组成的正极的可逆和不可逆容量损失来源。我们利用一个非典型的低电压切断(2.0 V vs. Li/Li+)来量化SE氧化还原的可逆性。使用慢速(5.5 mA gNMC-1)循环与>;在100小时的低压保持下,我们的电池达到了令人惊讶的96.2%的第一循环库仑效率,这比之前报道的要高(在调查的文献中,平均值:72%,最大值:91.6%)。我们澄清缓慢的NMC还原动力学在历史上被误认为是永久不可逆的容量损失。通过对损失机制的系统解耦,我们揭示了SE氧化还原的意外可逆性,并分离了导致容量损失的主要因素,概述了准确评估下一代SE材料和界面修改的策略。
Decoupling first-cycle capacity loss mechanisms in sulfide solid-state batteries†
Solid-state batteries (SSBs) promise more energy-dense storage than liquid electrolyte lithium-ion batteries (LIBs). However, first-cycle capacity loss is higher in SSBs than in LIBs due to interfacial reactions. The chemical evolution of key interfaces in SSBs has been extensively characterized. Electrochemically, however, we lack a versatile strategy for quantifying the reversibility of solid electrolyte (SE) redox for established and next-generation SSB electrolytes. In this work, we perform tailored electrochemical tests and operando X-ray diffraction to disentangle reversible and irreversible sources of capacity loss in positive electrodes composed of Li6PS5Cl SE, Li(Ni0.5Mn0.3Co0.2)O2 (NMC), and carbon conductive additives. We leverage an atypically low voltage cutoff (2.0 V vs. Li/Li+) to quantify the reversibility of SE redox. Using slow (5.5 mA gNMC−1) cycling paired with >100 h low-voltage holds, our cells achieve a surprising 96.2% first-cycle coulombic efficiency, which is higher than previously reported (mean: 72%, maximum: 91.6% across surveyed literature). We clarify that sluggish NMC relithiation kinetics have been historically mistaken for permanently irreversible capacity loss. Through systematic decoupling of loss mechanisms, we uncover the unexpected reversibility of SE redox and isolate the major contributors to capacity loss, outlining a strategy for accurate assessment of next-generation SE materials and interface modifications.
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).