Coherent‐Precipitation‐Stabilized Phase Formation in Over‐Stoichiometric Rocksalt‐Type Li Superionic Conductors
Year: 2024
Type: article
Abstract: Rationalizing synthetic pathways is crucial for material design and property optimization, especially for polymorphic and metastable phases. Over‐stoichiometric rocksalt (ORX) compounds, characterized by their face‐sharing configurations, are a promising group of materials with unique properties; however, their development is significantly hindered by challenges in synthesizability. Here, taking the recently identified Li superionic conductor, over‐stoichiometric rocksalt Li–In–Sn–O (o‐LISO) material as a prototypical ORX compound, the mechanisms of phase formation are systematically investigated. It is revealed that the spinel‐like phase with unconventional stoichiometry forms as coherent precipitate from the high‐temperature‐stabilized cation‐disordered rocksalt phase upon fast cooling. This process prevents direct phase decomposition and kinetically locks the system in a metastable state with the desired face‐sharing Li configurations. This insight enables us to enhance the ionic conductivity of o‐LISO to be >1 mS cm−1 at room temperature through low‐temperature post‐annealing. This work offers insights into the synthesis of ORX materials and highlights important opportunities in this new class of materials.
Source: Advanced Materials
Institutions: Lawrence Berkeley National Laboratory, University of California, Berkeley, Brookhaven National Laboratory, Pacific Northwest National Laboratory, Chinese Academy of Sciences, University of Chinese Academy of Sciences, University of Utah, Environmental Molecular Sciences Laboratory, Argonne National Laboratory, Florida State University
Language: English
Subfield: Electrical and Electronic Engineering
Field: Engineering
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $5,780
Funders: National Science Foundation, U.S. Department of Energy, U.S. Department of Commerce, Battelle, Washington State University, National Energy Research Scientific Computing Center, Office of Science, Office of Energy Efficiency and Renewable Energy, Basic Energy Sciences, Biological and Environmental Research, Vehicle Technologies Office, Office of Energy Efficiency, Argonne National Laboratory, Brookhaven National Laboratory, Lawrence Berkeley National Laboratory, Pacific Northwest National Laboratory
Awards: G102163711, G107546177, G1079818582, G1143651532, G1202769797, G122673668, G125460123, G1285306620, G1286236842, G1286251239, G1313983767, G1334204481, G1337544421, G138090931, G1677143136, G171842289, G1769256354, G1847291448, G1851334662, G1863003419, G1867732070, G1899721271, G2013908898, G223002938, G227997908, G2293800358, G241279073, G2506945562, G2510423872, G2638771445, G2710243964, G2820049545, G2857925935, G2988778103, G299733460, G30714459, G3075337988, G3083819904, G3262563802, G357145406, G391136020, G4158950854, G419881185, G426311843, G42916606, G429813595, G4501827968, MRI: Acquisition of a 400 MHz Nuclear Magnetic Resonance (NMR)Spectrometer to Enable Material Science Research, G4562702224, G495867719, G498139845, G5076365615, G5321382714, G5373841109, G5558627913, G5632581352, G5653134238, G5726405315, G5765906131, G613759197, G6330817128, G650090426, XSEDE: eXtreme Science and Engineering Discovery Environment, G6848031779, G6918803902, G6965541988, G7354628648, G7463374569, G7560550554, G7583137537, G7787287669, G8147674379, G821644656, G872144517, G8978062500, G969889393, G993149817
OpenAlex ID: W4405725232