Xia Yang, Li Jiaojiao, Xiao Zhen, Zhou Xiaozheng, Zhang Jun, Huang Hui, Gan Yongping, He Xinping, Zhang Wenkui
College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
Institute of Optoelectronic Materials and Devices, China Jiliang University, Hangzhou 310018, China.
ACS Appl Mater Interfaces. 2022 Jul 27;14(29):33361-33369. doi: 10.1021/acsami.2c08940. Epub 2022 Jul 14.
All-solid-state lithium batteries (ASSLBs) paired with an argyrodite sulfide solid electrolyte have become a candidate to take the world by storm for achieving high energy and safety. However, the undesirable interface design between a sulfide solid electrolyte and cathode is difficult to address its scalability production challenge. Particularly, the inferior interfacial contact between a sulfide solid electrolyte and cathode is an intractable obstacle for the large-scale commercial application of ASSLBs. Herein, an elaborately designed conformally in situ integration of a sulfide solid electrolyte onto a Ni-rich oxide cathode is proposed to overcome this issue through a facile tape casting method. In this unique integrated electrode structure, the sulfide solid electrolyte intimately makes contact with the Ni-rich oxide cathode, which significantly strengthens the solid-solid interfacial compatibility, as well as decreases the interfacial reaction resistances, thereby enabling rapid Li transportation and a stable interfacial structure. As a result, ASSLBs consisting of a sulfide solid electrolyte-integrated Ni-rich oxide cathode and Li anode exhibit high discharge capacity, excellent cyclic stability, and remarkable rate performance, which are superior to the cells with segregated structures composed of a Ni-rich oxide cathode, sulfide solid electrolyte, and Li anode. The features clearly indicate that the advanced interfacial contact between the cathode and solid electrolyte is responsible for ASSLBs with low polarization and fast reaction kinetics. Therefore, this work provides a rational proof-of-concept fabrication protocol for the reliable interfacial structure design of high-performance ASSLBs.
与硫银锗矿硫化物固体电解质配对的全固态锂电池（ASSLB）已成为有望在全球引发轰动以实现高能量和安全性的候选者。然而，硫化物固体电解质与阴极之间不理想的界面设计难以应对其规模化生产挑战。特别是，硫化物固体电解质与阴极之间较差的界面接触是ASSLB大规模商业应用的一个棘手障碍。在此，提出了一种精心设计的将硫化物固体电解质保形原位集成到富镍氧化物阴极上的方法，以通过简便的流延成型法克服这一问题。在这种独特的集成电极结构中，硫化物固体电解质与富镍氧化物阴极紧密接触，这显著增强了固 - 固界面兼容性，同时降低了界面反应电阻，从而实现快速的锂传输和稳定的界面结构。结果，由硫化物固体电解质集成的富镍氧化物阴极和锂阳极组成的ASSLB表现出高放电容量、优异的循环稳定性和出色的倍率性能，优于由富镍氧化物阴极、硫化物固体电解质和锂阳极组成的分离结构的电池。这些特性清楚地表明，阴极与固体电解质之间先进的界面接触是具有低极化和快速反应动力学的ASSLB的关键。因此，这项工作为高性能ASSLB可靠的界面结构设计提供了合理的概念验证制造方案。
