Lithium (Li) hosts, which can electrochemically accommodate Li in preformed pores of three-dimensional frameworks, have been investigated as an advanced electrode architecture for high-energy-density Li-metal batteries. However, most of the previous studies on Li hosts utilized electrochemically inert materials for their framework constituents, resulting in undesired loss of gravimetric/volumetric energy densities of the resulting batteries. Here, we present an electroactive Li host based on a microgrid-patterned Si electrode (denoted as the MPS host). The MPS host is fabricated using a microscale direct ink writing technique. The lithiophilicity, electronic conductivity, and porous structure of the MPS host are customized to ensure the preferential direction of Li-ion flux and electron conduction into the ordered pore space, while providing the redox capacity. The resulting MPS host enables stepwise sequential Si lithiation/delithiation (from the Si in the microgrid frameworks) and Li plating/stripping (inside the pore space between the microgrids) reactions, verifying its unique behavior as an electroactive Li host. In addition, a full cell assembled with the MPS host and the LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode (areal capacity = 3.8 mAh cm−2) exhibits high cell energy densities (644 Wh kgcell−1/1538 Wh Lcell−1) and reliable cyclability.
Bibliographical noteFunding Information:
This work was supported by the Basic Science Research Program (2021R1A2B5B03001615 and 2021M3D1A2043791) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and future planning, and the Technology Innovation Program (20012216) funded by the Ministry of Trade, Industry & Energy (MOTIE).
© 2022 The Royal Society of Chemistry
All Science Journal Classification (ASJC) codes
- Environmental Chemistry
- Renewable Energy, Sustainability and the Environment
- Nuclear Energy and Engineering