Chen Hao, Mai Xirong, Lin Xuqi, Wei Xiujuan, Li Meng, Huang Senchuan, Huang Zimo, Liang Yuhao, Zhang Shanqing
Institute for Sustainable Transformation, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou 510006, China.
Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center, Jieyang 515200, China.
ACS Appl Mater Interfaces. 2025 Oct 1;17(39):54905-54914. doi: 10.1021/acsami.5c13615. Epub 2025 Sep 23.
Li-rich layered manganese-based oxides (LRMOs) are promising high-capacity cathodes for next-generation lithium-ion batteries (LIBs). The challenges for commercialization are mainly rapid capacity fading and discharge voltage decay due to structural transformations, electrolyte decomposition, and transition-metal dissolution. Herein, we construct a robust multifunctional binding network to address these issues by combining two water-based polysaccharide binders, including guar gum (GG) and xanthan gum (XG). The XG-GG composite binder could build a robust hydrogen-bonded network to accommodate LRMO active materials, providing superior mechanical strength and adhesion, which is significantly superior to conventional poly(vinylidene difluoride) (PVDF). The binding network could prevent electrode cracking and active material loss during cycling. In particular, the polar functional groups in the binders could interact with the cathode surface and create a uniform protective cathode electrolyte interphase (CEI) and simultaneously adsorb dissolved transition-metal (TM) ions, suppressing their migration. LRMOs with the XG-GG binder exhibit significantly enhanced electrochemical performance, yielding a high initial capacity of 266.3 mAh/g, improved capacity retention (84.2% after 100 cycles at 1C), and suppressed average voltage decay. A full-cell configuration pairing an XG-GG-based Li-rich cathode with a graphite anode further demonstrates superior long-term stability. Our findings highlight that the establishment of a robust and functional binding network can synergistically overcome the mechanical and interfacial challenges of the high-energy LRMO cathodes and offer a sustainable, water-processable strategy for LIBs manufacturing.
富锂层状锰基氧化物（LRMO）是下一代锂离子电池（LIB）颇具前景的高容量正极材料。商业化面临的挑战主要是由于结构转变、电解质分解和过渡金属溶解导致的快速容量衰减和放电电压衰减。在此，我们通过结合两种水基多糖粘合剂，包括瓜尔胶（GG）和黄原胶（XG），构建了一个强大的多功能粘结网络来解决这些问题。XG - GG复合粘合剂可以构建一个强大的氢键网络来容纳LRMO活性材料，提供卓越的机械强度和粘附力，这明显优于传统的聚偏二氟乙烯（PVDF）。该粘结网络可以防止电极在循环过程中开裂和活性材料损失。特别是，粘合剂中的极性官能团可以与阴极表面相互作用，形成均匀的保护性阴极电解质界面（CEI），同时吸附溶解的过渡金属（TM）离子，抑制它们的迁移。采用XG - GG粘合剂的LRMO表现出显著增强的电化学性能，初始容量高达266.3 mAh/g，容量保持率提高（在1C下100次循环后为84.2%），平均电压衰减得到抑制。将基于XG - GG的富锂阴极与石墨阳极配对的全电池配置进一步证明了其卓越的长期稳定性。我们的研究结果突出表明，建立一个强大且功能性的粘结网络可以协同克服高能量LRMO阴极的机械和界面挑战，并为LIB制造提供一种可持续的、可水加工的策略。
