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With VULCAN’s help they monitored the low-conductivity phases’ formation during the thermal process, and found that it could be mitigated by doping the material—adding trace amounts of various elements that have high valences, or an affinity to create bonds, to reduce the effect. Being able to both suppress the formation of those unwanted phases and increase the number of useful vacancies for ion transport proved to be the key to unlocking garnets with high electrolytic performance.
“By tracking the lithium vacancies as functions of temperature and dopants, we found a common rule that the different dopants obey, and how they redistribute the vacancies in the framework of the garnets,” Chen said. “Furthermore, a comprehensive analysis of neutron diffraction results revealed how the dopants tune vacancy quantity, control vacancy distribution, and alter the charge carrier pathways in solid electrolytes.”
Thanks to the experiments by An and his team, materials researchers now have a proven method for achieving the best results in garnet structures—results that are sure to lead to safer materials with much needed savings of time and money.
“Now when people look at our work they can be guided how to make high ionic conductivity by choosing the right element with the right valence rather than repeatedly doing trial and error experiments on every single additional element—work that takes you a lot of time,” said An. “Now we can give you a simple formula to do it, and you should end up with a better material.”
Chen’s coauthors include Ezhiylmurugan Rangasamy, Chengdu Liang, Clarina R. dela Cruz, and Ke An. Related research of this material was conducted at the POWGEN instrument, SNS beam line 11A, using time of flight neutron diffraction data, and published in Advanced Energy Materials.
This work was sponsored by DOE’s Office of Science.
UT-Battelle manages ORNL for the DOE's Office of Science. The Office of Science is the single largest supporter of basic research in the physical sciences in the United States, and is working to address some of the most pressing challenges of our time.
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