Category: Publications

Our group has recently been invited to write a comprehensive review on computational studies of solid-state alkali conductivity in rechargeable alkali-ion batteries. This article has now been published in NPG Asia Materials! Check it out at http://www.nature.com/doifinder/10.1038/am.2016.7.

Iek-Heng Chu just published a new article in ACS Applied Materials & Interfaces. This is a highly collaborative work involving the expertise of many MAVRL group members as well as the Meng group. In this work, we investigate the performance limits of Li7P3S11, a highly promising lithium superionic conductor solid electrolyte. We find that Li7P3S11 is metastable at 0 K but becomes stable at above 630 K (∼360°C) when vibrational entropy contributions are accounted for, in agreement with differential scanning calorimetry measurements. Both scanning electron microscopy and the calculated Wulff shape show that Li7P3S11 tends to form relatively isotropic crystals. In terms of electrochemical stability, first-principles calculations predict that, unlike the LiCoO2 cathode, the olivine LiFePO4 and spinel LiMn2O4 cathodes are likely to form stable passivation interfaces with the Li7P3S11 SCE. This finding underscores the importance of considering multicomponent integration in developing an all-solid-state architecture. We also find that the AIMD-predicted room-temperature Li+ conductivity of 57 mS/cm is much higher than the experimental values suggesting the potential for further optimization.

Paul Lin published his first-author paper on the “Thermodynamics, Kinetics and Structural Evolution of ε-LiVOPO4 over Multiple Lithium Intercalation”in Chemistry of Materials, as well as his co-author paper in ACS Applied Materials & Interfaces on “Thermal Stability and Reactivity of Cathode Materials for Li-Ion Batteries”. These papers are collaborative work as part of the NorthEast Center for Chemical Energy Storage and focuses on multi-electron rechargeable battery cathodes that have the potential to yield much higher energy densities than traditional single-electron chemistries.

Congratulations to Zhuoying on her first paper in Chemistry of Materials title “Role of Na+ Interstitials and Dopants in Enhancing the Na+ Conductivity of the Cubic Na3PS4 Superionic Conductor”. In this work, we studied the effect of Na+ interstitials on the stability and ionic conductivity in the highly promising cubic Na3PS4 superionic conductor. We find that dopants significantly enhance the Na+ ionic conductivity and predict that Sn4+ doping may yield higher conductivities than previously achieved. The other authors are Iek-Heng Chu and Zhi Deng.

Zhi Deng, Zhenbin Wang and Iek-Heng Chu have just published their paper on “Elastic Properties of Alkali Superionic Conductor Electrolytes from First Principles Calculations” in the Journal of the Electrochemical Society. This work examines the elastic properties of ceramic alkali superionic conductor that are of interest in enabling safer, more energy dense all-solid-state batteries. Elastic properties have a critical influence on the fabrication, operation, and design of a battery.

Zhi Deng has just published his first paper titled “Rational Composition Optimization of the Lithium-Rich Li3OCl1–xBrx Anti-Perovskite Superionic Conductors” in Chemistry of Materials! In this work, we present a rational composition optimization strategy for maximizing the Li+ conductivity in the lithium-rich anti-perovskites (LRAPs) guided by a combination of first-principles calculations and percolation theory. We predict that the Li3OCl0.75Br0.25 to have a higher Li+ conductivity than Li3OCl0.5Br0.5, the highest conductivity LRAP identified experimentally thus far. These results highlight that there is scope for further enhancing the conductivity in the LRAP chemistry. The general approach developed can potentially be extended to other ion-conducting systems, such as the structurally similar perovskite oxygen-ion conductors of interest in solid-oxide fuel cells as well as other superionic conductors.