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@INPROCEEDINGS{Schierholz:1019737,
author = {Schierholz, Roland and Dzieciol, Krzysztof and Tempel,
Hermann and Kungl, Hans and Eichel, Rüdiger-A. and Zhang,
Qian},
title = {3{D}-microstructure of spindle-like {L}i1{T}i2({PO}4)3
particles revealed by electron microscopy},
reportid = {FZJ-2023-05568},
year = {2023},
abstract = {1. Introduction Pure Li1Ti2(PO4)3 (LTP) is an anode
material with NASICON structure and a lithiation potential
of 2.31 V.[1] This potential fits the electrochemical
stability window of the promising isostructural solid state
electrolyte Li1+xAlxTi2-x(PO4)3 (LATP, which is obtained by
trivalent substitution and application in an all-phosphate
solid state battery has been demonstrated.[2] Comparison of
different synthesis methods revealed an enhanced cycling
performance of solvothermally prepared LTP with spindle-like
particles of 2 – 5 µm size compared to the same material
prepared by sol-gel based Pecchini method.[3] 2.
ObjectivesScanning electron microscopy (SEM) suggests that
spindle-like particles are formed by sub particles of about
300 nm size, but as only the surface is accessible by SEM
the origin of the enhanced performance remains unclear. With
focused ion beam (FIB) and (Scanning) Transmission Electron
Microscopy the inner volume can be characterized to give a
complete picture of the particles crystal and microstructure
as well as its local chemical composition. 3. Materials and
methodsThe particles were synthesized by solvothermal
reaction, consecutively vacuum dried and annealed at 800
°C.[3] These particles were then dispersed in ethanol and a
droplet was put on a silicon wafer for FIB-SEM experiments.
FIB tomography and TEM-lamella preparation were conducted
with a Helios Nanolab 460F1, FEI, Netherlands.[4] TEM and
STEM analysis was conducted in a Tecnai F20 and a Titan G2
Crewley.[5]4. ResultsSEM imaging shows the morphology, with
sub particles forming a dumbbell like particle, and already
provides hints for the presence of two secondary phases, on
nanoparticles, the other a bulky phase with different
surface morphology. The presence oof different phases is
approved by chemical contrast in BSE-images of cross
sections and STEM HAADF imaging. STEM-EDS gives an estimate
of the chemical compositions which is completed by STEM-EELS
for the detection of Lithium. HRTEM and HRSTEM could then
identify the crystallographic structures of these secondary
phases to be TiO2 anatase for the nanoparticles and LiTiPO5
(Pnma ICSD #153522) for the bulky secondary phase.
FIB-tomography revealed that the majority of the TiO2
nanoparticles are interconnected.5. ConclusionsThe complex
microstructure of the spindle-like LTP particles can only be
solved by a combination of FIB-tomography and STEM-analysis.
The three-dimensional network of TiO2-nanoparticles seem to
improve the cycling behavior, as it may enhance the
diffusion and can also contribute to capacity and is no dead
material.[6] [1] S. Yu et al., ACS Appl. Mater. Interfaces
(2018) Vol. 10, No. 26 p. 22264-22277
https://doi.org/10.1021/acsami.8b05902 [2] H. Aono et al.,
Journal of The Electrochemical Society , (1990) 137, 4, p.
1023-1027 https://doi.org/10.1149/1.2086597 [3] S. Yu et
al., ChemElectroChem (2016) Vol. 3, No. 7, p. 1157-1169
https://doi.org/10.1002/celc.201600125 [4] M. Kruth et al.,
Journal of large-scale research facilities JLSRF (2016) 2,
A59 https://doi.org/10.17815/jlsrf-2-105 [5] A. Kovács et
al., Journal of large-scale research facilities JLSRF (2016)
2, A43 https://doi.org/10.17815/jlsrf-2-68 [6] M. Madian et
al., Batteries (2018) 4, 7,
https://doi.org/10.3390/batteries4010007 [7] M.L. Sushko
Mechanism of Li+/Electron Conductivity in Rutile and Anatase
TiO2 Nanoparticles J. Phys. Chem. C , (2012) 114, 47
American Chemical Society, p. 20277-20283
https://doi.org/10.1021/jp107982c Figure 1: SEM-BSE image of
a typical spindle-like LTP-particle.},
month = {Feb},
date = {2023-02-26},
organization = {Microscopy Conference, Darmstadt
(Germany), 26 Feb 2023 - 2 Mar 2023},
subtyp = {Other},
cin = {IEK-9},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {1121 - Digitalization and Systems Technology for
Flexibility Solutions (POF4-112)},
pid = {G:(DE-HGF)POF4-1121},
typ = {PUB:(DE-HGF)24},
url = {https://juser.fz-juelich.de/record/1019737},
}