Recently, Prof. Linsen LI and Prof. Zifeng MA at School of Chemistry and Chemical Engineering of Shanghai Jiao Tong University (SJTU) collaborated with Prof. Venkatasubramanian Viswanathan at Carnegie Mellon University (CMU) and Prof. Yet-Ming Chiang at Massachusetts Institute of Technology (MIT), and published an article titled Design Principles for Self-forming Interfaces Enabling Stable Lithium Metal Anodes on Proceedings of the National Academy of Sciences of the United States of America. Yingying ZHU, a doctoral student at SJTU and Vikram Pande at CMU are co-first authors of the article.


Li-ion batteries have been widely used in mobile electronics, electric cars, and energy storage power stations. Matching high-voltage oxide cathodes (>4V vs. Li+/ Li) with thin lithium (Li) metal (<50 μm in thickness) anodes promises Li-ion batteries with specific energies exceeding 350 watt hours (Wh) kg−1, higher than that of graphite anodes（~300 Wh/kg, ~750 Wh/L）.


However, the cycle life of thin Li-metal anodes is severely limited by short-circuits (i.e., “sudden death”) caused by Li-dendrite formation and low coulombic efficiency (CE) as a result of side reactions between Li metal and electrolyte (i.e., “gradual death”). The former two conditions are both closely linked to the morphology and the surface area of Li-metal particles.


The key to prolong the cycle life of Li-metal rechargeable batteries is to change the crystal growth behavior of Li-metal in the electrochemical deposition process, inducing the production of Li-metal particles with large size and small specific surface area and promoting dense deposition. This could be achieved by regulating the properties of SEI. This work has established clear design principles for self-forming interfaces enabling stable Li-metal anodes by combing experiments and DFT simulations and analysis. 


This work has elucidated the correlation among properties of SEI, electrochemical deposition behavior of Li-metal and CE and established design principles for well-functioning SEI to improve the performance of Li-metal rechargeable batteries.


This work was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the US DOE through Advanced Battery Materials Research Program Contract DE-EE0007810, and supported by the start-up fund of the Shanghai Jiao Tong University and the Natural Science Foundation of Shanghai, the Science and Technology Commission Shanghai Municipality (Grant 19ZR1475100; to L.S.L).

Translator: Chenyun SUN

Reviser: Xiaoke HU