The inability to guide the nucleation locations of electrochemically deposited Li has long been considered the main factor limiting the utilization of high-energy-density Li-metal batteries. In this study, an electrical conductivity gradient interfacial host comprising 1D high conductivity copper nanowires and nanocellulose insulating layers is used in stable Li-metal anodes. The conductivity gradient system guides the nucleation sites of Li-metal to be directed during electrochemical plating. Additionally, the controlled parameter of the intermediate layer affects the highly stable Li-metal plating. The electrochemical behavior is confirmed through experiments associated with the COMSOL Multiphysics simulation data. The distributed Li-ion reaction flux resulting from the controlled electrical conductivity enables stable cycling for more than 250 cycles at 1 mA cm−2. The gradient system effectively suppresses dendrite growth even at a high current density of 5 mA cm−2 and ensures Li plating and stripping with ultra-long-term stability. To demonstrate the high-energy-density full-cell application of the developed anode, it is paired with the LiNi0.8Co0.1Mn0.1O2 cathode. The cells demonstrate a high capacity retention of 90% with an extremely high Coulombic efficiency of 99.8% over 100 cycles. These results shed light on the formidable challenges involved in exploiting the engineering aspects of high-energy-density Li-metal batteries.
Bibliographical noteFunding Information:
This work was supported by the Basic Science Research Program (2017M1A2A2044501, 2018R1A2A1A05019733, 2018M3D1A1058624, and 2019R1A2C2002996), Wearable Platform Materials Technology Center (2016R1A5A1009926), Future Materials Discovery Program (2016M3D1A1027831), Basic Research Lab Program (2017R1A4A1015533), and Technology Development Program to Solve Climate Changes (2018M1A2A2063341) through the National Research Foundation of Korea (NRF) funded by the Ministry of Science, ICT and Future Planning.
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All Science Journal Classification (ASJC) codes
- Materials Science(all)
- Condensed Matter Physics