High-energy all-solid-state lithium batteries enabled by Co-free LiNiO2 cathodes with robust outside-in structures

Citation:

Longlong Wang, Mukherjee, Ayan , Kuo, Chang-Yang , Chakrabarty, Sankalpita , Yemini, Reut , Dameron, Arrelaine A, DuMont, Jaime W, Akella, Sri Harsha , Saha, Arka , Taragin, Sarah , Aviv, Hagit , Naveh, Doron , Sharon, Daniel , Chan, Ting-Shan , Lin, Hong-Ji , Lee, Jyh-Fu , Chen, Chien-Te , Liu, Boyang , Gao, Xiangwen , Basu, Suddhasatwa , Hu, Zhiwei , Aurbach, Doron , Bruce, Peter G. , and Noked, Malachi . 2024. “High-Energy All-Solid-State Lithium Batteries Enabled By Co-Free Linio2 Cathodes With Robust Outside-In Structures”. Nature Nanotechnology, 19, 2, Pp. 208 - 218. https://www.nature.com/articles/s41565-023-01519-8.

Abstract:

A critical current challenge in the development of all-solid-state lithium batteries (ASSLBs) is reducing the cost of fabrication without compromising the performance. Here we report a sulfide ASSLB based on a high-energy, Co-free LiNiO2 cathode with a robust outside-in structure. This promising cathode is enabled by the high-pressure O2 synthesis and subsequent atomic layer deposition of a unique ultrathin LixAlyZnzOδ protective layer comprising a LixAlyZnzOδ surface coating region and an Al and Zn near-surface doping region. This high-quality artificial interphase enhances the structural stability and interfacial dynamics of the cathode as it mitigates the contact loss and continuous side reactions at the cathode/solid electrolyte interface. As a result, our ASSLBs exhibit a high areal capacity (4.65 mAh cm−2), a high specific cathode capacity (203 mAh g−1), superior cycling stability (92% capacity retention after 200 cycles) and a good rate capability (93 mAh g−1 at 2C). This work also offers mechanistic insights into how to break through the limitation of using expensive cathodes (for example, Co-based) and coatings (for example, Nb-, Ta-, La- or Zr-based) while still achieving a high-energy ASSLB performance.