Interface Limited Lithium Transport in Solid-State Batteries.
Understanding the role of interfaces is important for improving the performance of all-solid-state lithium ion batteries. To study these interfaces, we present a novel approach for fabrication of electrochemically active nanobatteries using focused ion beams and their characterization by analytical electron microscopy. Morphological changes by scanning transmission electron microscopy imaging and correlated elemental concentration changes by electron energy loss spectroscopy mapping are presented. We provide first evidence of lithium accumulation at the anode/current collector (Si/Cu) and cathode/electrolyte (LixCoO2/LiPON) interfaces, which can be accounted for the irreversible capacity losses. Interdiffusion of elements at the Si/LiPON interface was also witnessed with a distinct contrast layer. These results highlight that the interfaces may limit the lithium transport significantly in solid-state batteries. Fabrication of electrochemically active nanobatteries also enables in situ electron microscopy observation of electrochemical phenomena in a variety of solid-state battery chemistries.
†Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States.
Dhamodaran
D
Santhanagopalan
†Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States.
Danna
D
Qian
†Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States.
Thomas
T
McGilvray
†Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States.
Ziying
Z
Wang
‡Brookhaven National Laboratory, Upton, New York 11973, United States.
Feng
F
Wang
‡Brookhaven National Laboratory, Upton, New York 11973, United States.
Fernando
F
Camino
‡Brookhaven National Laboratory, Upton, New York 11973, United States.
Jason
J
Graetz
§Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States.
Nancy
N
Dudney
†Department of NanoEngineering, University of California, San Diego, 9500 Gilman Drive, La Jolla, California 92093, United States.
Ying Shirley
YS
Meng
STEM-EELS; electrochemistry; focused ion beams; interface; solid-state nanobattery