Abstract
The universal cathode crossover such as chemical and oxygen has been significantly overlooked in lithium metal batteries using high-energy cathodes which leads to severe capacity degradation and raises serious safety concerns. Herein, a versatile and thin (≈25 μm) interlayer composed of multifunctional active sites was developed to simultaneously regulate the Li deposition process and suppress the cathode crossover. The as-induced dual-gradient solid-electrolyte interphase combined with abundant lithiophilic sites enable stable Li stripping/plating process even under high current density of 10 mA cm−2. Moreover, X-ray photoelectron spectroscopy and synchrotron X-ray experiments revealed that N-rich framework and CoZn dual active sites can effectively mitigate the undesired cathode crossover, hence significantly minimizing Li corrosion. Therefore, assembled lithium metal cells using various high-energy cathode materials including LiNi0.7Mn0.2Co0.1O2, Li1.2Co0.1Mn0.55Ni0.15O2, and sulfur demonstrate significantly improved cycling stability with high cathode loading.
| Original language | English |
|---|---|
| Article number | e202217476 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 62 |
| Issue number | 19 |
| DOIs | |
| State | Published - May 2 2023 |
| Externally published | Yes |
Funding
Research at the Hong Kong Polytechnic University was funded by research grants from Shenzhen Science and Technology Program (SGDX20190816230615451), the Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515110798), GDSTC‐Guangdong‐HK‐Macao Joint Laboratory for Photonic‐Thermal‐Electrical Energy Materials and Devices (GDSTC No. 2019B121205001). Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from Tien Duong of the US DOE's Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS), an Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE‐AC02‐06CH11357. G.X. and K.A. thank the Clean Vehicle Consortium, US, China Clean Energy Research Centre (CERC‐CVC2) for support. Research at the Hong Kong Polytechnic University was funded by research grants from Shenzhen Science and Technology Program (SGDX20190816230615451), the Guangdong Basic and Applied Basic Research Foundation (No. 2020A1515110798), GDSTC-Guangdong-HK-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices (GDSTC No. 2019B121205001). Research at the Argonne National Laboratory was funded by the US Department of Energy (DOE), Vehicle Technologies Office. Support from Tien Duong of the US DOE's Office of Vehicle Technologies Program is gratefully acknowledged. Use of the Advanced Photon Source (APS), an Office of Science user facilities, was supported by the US Department of Energy, Office of Science and Office of Basic Energy Sciences, under contract no. DE-AC02-06CH11357. G.X. and K.A. thank the Clean Vehicle Consortium, US, China Clean Energy Research Centre (CERC-CVC2) for support.
Keywords
- Cathode Cross-over
- High-Energy Cathode
- Lithium-Metal Batteries
- Solid-Electrolyte Interphase