Fan Ziqiang, Zhou Xunzhu, Qiu Jingwei, Yang Zhuo, Lei Chenxi, Hao Zhiqiang, Li Jianhui, Li Lin, Zeng Ronghua, Chou Shu-Lei
Department Institute for Carbon Neutralization, College of Chemistry and Materials Engineering, Wenzhou University, Wenzhou, Zhejiang 325035, China.
Department National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs, Engineering Research Center of MTEES (Ministry of Education), Key Laboratory of ETESPG (GHEI), School of Chemistry, South China Normal University, Guangzhou, Guangdong 510006, China.
Angew Chem Int Ed Engl. 2023 Sep 25;62(39):e202308888. doi: 10.1002/anie.202308888. Epub 2023 Aug 21.
High-voltage lithium-ion batteries (LIBs) have attracted great attention due to their promising high energy density. However, severe capacity degradation is witnessed, which originated from the incompatible and unstable electrolyte-electrode interphase at high voltage. Herein, a robust additive-induced sulfur-rich interphase is constructed by introducing an additive with ultrahigh S-content (34.04 %, methylene methyl disulfonate, MMDS) in 4.6 V LiNi Co Mn O (NCM523)||graphite pouch cell. The MMDS does not directly participate the inner Li sheath, but the strong interactions between MMDS and PF anions promote the preferential decomposition of MMDS and broaden the oxidation stability, facilitating the formation of an ultrathin but robust sulfur-rich interfacial layer. The electrolyte consumption, gas production, phase transformation and dissolution of transition metal ions were effectively inhibited. As expected, the 4.6 V NCM523||graphite pouch cell delivers a high capacity retention of 87.99 % even after 800 cycles. This work shares new insight into the sulfur-rich additive-induced electrolyte-electrode interphase for stable high-voltage LIBs.
高压锂离子电池（LIBs）因其有望实现的高能量密度而备受关注。然而，人们观察到严重的容量衰减，这源于高压下不相容且不稳定的电解质-电极界面。在此，通过在4.6 V锂镍钴锰氧化物（NCM523）||石墨软包电池中引入超高硫含量（34.04 %）的添加剂（亚甲基甲基二磺酸酯，MMDS），构建了一种由添加剂诱导的坚固富硫界面。MMDS并不直接参与内部锂鞘层的形成，但MMDS与PF阴离子之间的强相互作用促进了MMDS的优先分解并拓宽了氧化稳定性，有助于形成超薄但坚固的富硫界面层。电解质消耗、气体产生、相变以及过渡金属离子的溶解均得到有效抑制。正如预期的那样，即使经过800次循环，4.6 V NCM523||石墨软包电池仍具有87.99 %的高容量保持率。这项工作为稳定的高压LIBs中富硫添加剂诱导的电解质-电极界面提供了新的见解。
