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Today I sucessfully defended my PhD thesis "Molecular Elucidation of Reaction Mechanisms in Aluminum and Lithium Metal Batteries by Solid-State NMR Spectroscopy and Electrochemical Methods". My PhD journey has been a greatly enjoyable 5 years and I have far too many people to thank for getting me to this point. However, I must acknowledge my committee members, Prof. Alex Couzis, Prof. Ruth Stark, Prof. George John, Prof. Elizabeth Biddinger, and my advisor Prof. Robert Messinger for their great support today. Special thanks to Rob for all the hard work we put in together!
The latest work from our group "Reversible Zinc Electrodeposition at −60 ℃ Using a Deep Eutectic Electrolyte for Low-Temperature Zinc Metal Batteries" was published today. In this work we demonstrate an electrolyte with a deep-eutectic point to enable reversible zinc electrodeposition down to temperatures of -60 ℃. We make electrolytes in different ratios of [EMIm]TFSI with gamma-butyrolactone (GBL) which are probed electrochemically to determine their macroscopic properties, and further analysed at the molecular level via NMR spectroscopy and molecular dynamics (MD) simulations to explain the differences in performance from an atomistic approach.
Our new study of aluminium-organic batteries, entitled "Revealing Impacts of Electrolyte Speciation on Ionic Charge Storage in Aluminum-Quinone Batteries by NMR Spectroscopy", is now out in the Journal of Magnetic Resonance. This is a detailed analysis of the ionic charge storage mechanisms in aluminium-quinone batteries where we begin by detailing the speciation of three different Lewis acidic ionic liquid or ionic liquid analogue electrolytes by liquid-state NMR, we then use solid-state NMR to determine the nature of the complexed ions upon electrochemical discharge in each electrolyte. We further use DFT calculations to both determine the most favorable electroactive cation generation pathways and to link the experimentally derived NMR quadrupolar parameters to a physical basis of ion interaction with different quinone structures. Finally, we also validate our hypothesised mechanisms with targeted experiments, proving the function of various ionic species.