Hume-Rothery Symposium on First-Principles Materials Design: Interface First-principle Method with Experiments I
Sponsored by: TMS Functional Materials Division, TMS Structural Materials Division, TMS: Alloy Phases Committee
Program Organizers: Bin Ouyang, Florida State University; Mark Asta, University of California, Berkeley; Geoffroy Hautier, Dartmouth College; Wei Xiong, University of Pittsburgh; Anton Van der Ven, University of California, Santa Barbara
Wednesday 8:30 AM
March 22, 2023
Room: Cobalt 501C
Location: Hilton
Session Chair: Hailong Chen, Georgia Institute of Technology; Raphaele Clement, University of California, Santa Barbara
8:30 AM Invited
Predicting Synthesis and Synthesizability Beyond the DFT Convex Hull: Wenhao Sun1; 1University of Michigan
The computational materials discovery pipeline often remains bottlenecked by the difficulty of synthesizing predicted compounds in the lab. To realize the vision of accelerated materials design, a quantitative and predictive theory of materials synthesis is urgently needed. From a theoretical perspective, three guiding questions for predictive synthesis are: 1) Which compounds designed in silico can be synthesized? 2) For a computationally-designed material, which materials synthesis method—e.g. solid-state, hydrothermal, vapor deposition, etc.—is best to synthesize it? 3) Within the parameter space of that synthesis method, what synthesis ‘recipe’ can lead to a phase-pure synthesis of the predicted compound? I will illustrate how careful consideration of the local thermodynamic conditions where materials nucleate can help us anticipate which stable or metastable phases which may form during synthesis. Guided by these insights, solid-state chemists can more rationally navigate the thermodynamic and kinetic energy landscape towards the targeted synthesis of desired materials.
9:00 AM Invited
New Battery Chemistry from Conventional Layered Cathode Materials for Advanced Lithium-ion Batteries: Ki Suk Kang1; 1Seoul National University
For the past decades, extensive efforts have been placed in improving the performance of the layered compounds for cathodes such as by compositional tuning and structural modifications. One of the notable approaches in recent years is to adopt excess amounts of lithium-ions in the layered materials, which surprisingly revealed that the specific capacity can be boosted in the layered cathodes via the shift from the conventional cationic redox reaction relying on transition metals (Co, Ni and Mn) to the cumulative cationic and anionic (oxygen) redox reaction. In this journey to explore the ‘lithium-excess layered cathodes’, various new findings have been being disclosed. In this talk, I will present our recent understandings on these materials with respect to the lithium insertion mechanism that differs from what have been observed in conventional layered materials and the effect of the layered stacking sequences, and discuss on the outlook on the lithium-excess layered cathodes.
9:30 AM Invited
Dynamic Stability Design of Materials for Solid-state Batteries: Xin Li1; 1Harvard University
Solid state battery in operation is a dynamically coupled device under local mechanical constriction. The growth of lithium dendrite and crack in battery cycling can be stopped by self-limited local decompositions between lithium dendrite and certain solid electrolytes, enabling the battery to be cycled at high current densities. The functional decomposition here is a type of dynamic stability, which needs a delicate balance of sufficient decomposition energy to generate the decomposition and appropriate self-limiting ability to passivate it. We thus constructed a constrained ensemble computational platform to describe the unique local environment under mechanical constriction. High-throughput computation was then used to collect the two metrics for describing the dynamic stability under constrained ensemble, by also utilizing the ab initio data for all the inorganic materials in the Materials Project. Machine learning was used to extract the correlation between material composition and dynamic stability for the design of new solid electrolytes.
10:00 AM Break
10:20 AM Invited
Establishing Links between Synthesis, Defect Landscape, and Ion Conduction in Halide-type Solid Electrolytes: Raphaele Clement1; 1University of California, Santa Barbara
Rocksalt-type halide electrolytes have spurred interest over the past few years due to their high ionic conductivities and stability against high voltage cathodes. While their conduction properties depend sensitively on synthesis conditions, these materials constitute a challenge for characterization. I will show that a combination of synchrotron XRD, NMR, and first principles and molecular dynamics simulations, allows us to determine the origin of high ion conduction, providing key design principles for this family of electrolytes. Our work has revealed that the high conductivity of ball-milled Li3YCl6 stems from the presence of stacking faults in the rocksalt-type structure.[1] Exploring Na3-xY1-xZrxCl6 compounds, we have again found that disorder facilitates ionic diffusion in mixed Y/Zr compositions[2,3], while conduction is affected by polymorphism in Na3YCl6 and Na2ZrCl6. [1] Sebti et al., J. Am. Chem. Soc., 144, 5795 (2022). [2] Wu et al., Nat. Commun., 12(1), 1256 (2021).[3] Sebti et al., in preparation.