Engineering Stable Anode-Free Architectures for Solid-State Batteries
Anode-free all-solid-state batteries (ASSBs) offer an exciting route to ultra–high energy density and safer rechargeable systems, but their development is hindered by challenges such as uneven lithium nucleation, dendritic growth, and interfacial delamination.
Our group addresses these issues through architectural and interfacial design strategies that precisely control lithium deposition. We uncovered a pore-size-dependent creep mechanism that dictates how lithium infiltrates 3D porous hosts, providing clear rules for building robust anode frameworks. We also introduced the concept of a magnesium breathing anode, in which a lithium concentration gradient drives uniform lithiation and stable expansion contraction, enabling exceptionally long cycling stability at room temperature. By linking the fundamental mechanics of lithium growth with practical anode design, our research lays the groundwork for safe, durable, and commercially viable anode-free ASSBs bridging materials science, electrochemistry, and device engineering.
Dayoung Jun‡, Se Hwan Park‡, Ji Eun Jung, Seong Gyu Lee, Kyu Seok Kim, Ji Young Kim, Ki Yoon Bae, Samick Son, Yun Jung Lee*, Ultra-Stable Breathing Anode for Li-Free All-Solid-State Battery Based on Li Concentration Gradient in Magnesium Particles, Advanced Functional Materials, 34(8), 2310259, 2023
Se Hwan Park, Dayoung Jun, Gyu Hyeon Lee, Seong Gyu Lee, Ji Eun Jung, Ki Yoon Bae, Samick Son, and Yun Jung Lee*, Designing 3D Anode Based on Pore-Size-Dependent Li Deposition Behavior for Reversible Li-Free All-Solid-State Batteries, Advanced Science, 9, 2203130, 2022
Material–Interface Co-Design for Stable Anodes
All-solid-state batteries promise high energy density and safety, yet Li-metal instability at the anode side limits durability. We advance anodeless architectures through materials and interface design. First, sonochemically grown MgF₂ nanodots on carbon convert to a Mg–Li alloy and LiF, lowering overpotential and enabling uniform plating (81.4% after 200 cycles, 30 °C). Second, thermally reduced Ag-ion complexes yield well-dispersed Ag/C interlayers that act as mixed ionic–electronic conductors, supporting compact Li deposition with 91% retention after 500 cycles and low-pressure pouch validation. Third, we establish porous-interlayer design rules: adhesion work determines where Li forms, while pore size, temperature, scaffold, and Ag lithiophilicity drive Coble-creep transport to the interlayer–collector interface, minimizing contact with sulfide electrolytes. Together, these strategies stabilize Li deposition and move anodeless ASSBs toward practical, large-format cells.
Sang-Jin Jeon‡, Chihyun Hwang‡, Hyun-Seung Kim‡, Jonghyun Park, Jang-Yeon Hwang, Yijin Jung, Ran Choi, Min-Sang Song, Yun Jung Lee*, Ji-Sang Yu*, Yun-Chae Jung*, Sonochemically Prepared Nanodot Magnesium Fluoride-Based Anodeless Carbon Substrate for Simultaneously Reinforcing Interphasial and Reaction Kinetics for Sulfide-Based All-Solid-State Batteries, Advanced Energy Materials, 14(45), 2402887, 2024
Yun-Chae Jung, Chihyun Hwang, Myung-Jun Kwaw, Sang-Jin Jeon, Yun Jung Lee, Won-Jin Kwak, Hyun-Seung Kim, KyungSu Kim, Woosuk Cho*, Ji-Sang Yu*, On-site formation of silver decorated carbon as an anodeless electrode for high-energy density all-solid-state batteries, Journal of Materials Chemistry A, 11, 25275-25282, 2023
Se Hwan Park‡, Dayoung Jun‡, Ji Eun Jung, Seong Gyu Lee, Gyu Hyeon Lee, Yun Jung Lee*, Clarification of Li Deposition Behavior on Anodes with a Porous Interlayer in Li-free All-Solid-State Batteries, Journal of Materials Chemistry A, 10, 21995-22006, 2022