Premium
Interfacial Ion‐Transport Mechanism of Li 7 (Al 0.1 )La 3 Zr 2 O 12 Solid Electrolyte Modified by using a Spark Plasma Sintering Method
Author(s) -
Bai Lixiong,
Xue Wendong,
Xue Yawen,
Qin Haixia,
Li Yan,
Li Yong,
Sun Jialin
Publication year - 2018
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.201801229
Subject(s) - grain boundary , spark plasma sintering , materials science , electrolyte , lithium (medication) , scanning electron microscope , sintering , analytical chemistry (journal) , grain size , ionic conductivity , ion , transmission electron microscopy , fast ion conductor , composite material , microstructure , nanotechnology , chemistry , electrode , medicine , chromatography , endocrinology , organic chemistry
A novel interfacial in situ modification for Li 7 (Al 0.1 )La 3 Zr 2 O 12 is designed and prepared by using a spark plasma sintering method. The modified interface with most grain boundary area exhibits excellent interfacial electrochemical properties. The X‐ray diffraction (XRD) and scanning electron microscope (SEM) data indicate that the interfacial modified specimen (spark plasma sintering method, 1000 °C, 5 min) with 38.2(6) nm grain diameter and 32,134 cm 2 /g grain boundary specific surface area has the highest ionic conductivity (8.84×10 −4 S/cm −1 ). The lithium‐ion transmission mechanism in grain‐internal and grain boundaries is revealed by ab initio theory, using Materials Studio software. Furthermore, the first‐principles calculation data indicate that the migration barrier of Li + at the Li 7 (Al 0.1 )La 3 Zr 2 O 12 solid electrolyte grain boundary is 0.21 eV, which is only 2/3 of that in the grain internal (0.33 eV). As a result, SPS interfacial in situ processing technology can increase the grain boundary area, thereby reducing the ion transport barrier and the interfacial impedance of the material.