Abstract
Lithium lanthanum zirconate (LLZO) is a promising Li+ ion conductor for applications as a ceramic solid electrolyte in all-solid-state lithium batteries. However, the tetragonal and cubic phases of LLZO differ in lithium ionic conductivity by several orders of magnitude with extrinsic dopants or nanostructuring often required to stabilize the high conductivity cubic phase at room temperature. Here, we show that nanostructured LLZO can be prepared by templating onto various cellulosic fibers, including laboratory Kimwipes, Whatman filter paper, and nanocellulose fibrils, followed by calcination at 700-800 °C. The effect of templating material, calcination temperature, calcination time, and heating ramp rate on the LLZO crystal structure and morphology were thoroughly investigated. Templating was determined to be an effective method for controlling the LLZO size and morphology, and low calcination times and ramp rates were found to favor the formation of small ligaments. Furthermore, it was verified that cubic phase stabilization occurred for LLZO with ligaments of size less than 1 μm on average without the use of extrinsic dopants. This work provides more information regarding the size dependence of cubic LLZO stabilization that was not previously investigated in detail, and cellulosic templating is shown to be a viable route toward the scalable, sustainable synthesis of LLZO solid electrolytes.
| Original language | English (US) |
|---|---|
| Pages (from-to) | 6391-6398 |
| Number of pages | 8 |
| Journal | ACS Sustainable Chemistry and Engineering |
| Volume | 4 |
| Issue number | 12 |
| DOIs | |
| State | Published - Dec 5 2016 |
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Keywords
- Li-ion batteries
- Lithium lanthanum zirconate
- Nanocellulose
- Solid electrolyte
- Templating
ASJC Scopus subject areas
- Chemistry(all)
- Environmental Chemistry
- Chemical Engineering(all)
- Renewable Energy, Sustainability and the Environment
Cite this
Preparation of Nano- and Microstructured Garnet Li7La3Zr2O12 Solid Electrolytes for Li-Ion Batteries via Cellulose Templating. / Gordon, Zachary D.; Yang, Ting; Gomes Morgado, Guilherme Bruno; Chan, Candace.
In: ACS Sustainable Chemistry and Engineering, Vol. 4, No. 12, 05.12.2016, p. 6391-6398.Research output: Contribution to journal › Article
}
TY - JOUR
T1 - Preparation of Nano- and Microstructured Garnet Li7La3Zr2O12 Solid Electrolytes for Li-Ion Batteries via Cellulose Templating
AU - Gordon, Zachary D.
AU - Yang, Ting
AU - Gomes Morgado, Guilherme Bruno
AU - Chan, Candace
PY - 2016/12/5
Y1 - 2016/12/5
N2 - Lithium lanthanum zirconate (LLZO) is a promising Li+ ion conductor for applications as a ceramic solid electrolyte in all-solid-state lithium batteries. However, the tetragonal and cubic phases of LLZO differ in lithium ionic conductivity by several orders of magnitude with extrinsic dopants or nanostructuring often required to stabilize the high conductivity cubic phase at room temperature. Here, we show that nanostructured LLZO can be prepared by templating onto various cellulosic fibers, including laboratory Kimwipes, Whatman filter paper, and nanocellulose fibrils, followed by calcination at 700-800 °C. The effect of templating material, calcination temperature, calcination time, and heating ramp rate on the LLZO crystal structure and morphology were thoroughly investigated. Templating was determined to be an effective method for controlling the LLZO size and morphology, and low calcination times and ramp rates were found to favor the formation of small ligaments. Furthermore, it was verified that cubic phase stabilization occurred for LLZO with ligaments of size less than 1 μm on average without the use of extrinsic dopants. This work provides more information regarding the size dependence of cubic LLZO stabilization that was not previously investigated in detail, and cellulosic templating is shown to be a viable route toward the scalable, sustainable synthesis of LLZO solid electrolytes.
AB - Lithium lanthanum zirconate (LLZO) is a promising Li+ ion conductor for applications as a ceramic solid electrolyte in all-solid-state lithium batteries. However, the tetragonal and cubic phases of LLZO differ in lithium ionic conductivity by several orders of magnitude with extrinsic dopants or nanostructuring often required to stabilize the high conductivity cubic phase at room temperature. Here, we show that nanostructured LLZO can be prepared by templating onto various cellulosic fibers, including laboratory Kimwipes, Whatman filter paper, and nanocellulose fibrils, followed by calcination at 700-800 °C. The effect of templating material, calcination temperature, calcination time, and heating ramp rate on the LLZO crystal structure and morphology were thoroughly investigated. Templating was determined to be an effective method for controlling the LLZO size and morphology, and low calcination times and ramp rates were found to favor the formation of small ligaments. Furthermore, it was verified that cubic phase stabilization occurred for LLZO with ligaments of size less than 1 μm on average without the use of extrinsic dopants. This work provides more information regarding the size dependence of cubic LLZO stabilization that was not previously investigated in detail, and cellulosic templating is shown to be a viable route toward the scalable, sustainable synthesis of LLZO solid electrolytes.
KW - Li-ion batteries
KW - Lithium lanthanum zirconate
KW - Nanocellulose
KW - Solid electrolyte
KW - Templating
UR - http://www.scopus.com/inward/record.url?scp=85003011290&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85003011290&partnerID=8YFLogxK
U2 - 10.1021/acssuschemeng.6b01032
DO - 10.1021/acssuschemeng.6b01032
M3 - Article
AN - SCOPUS:85003011290
VL - 4
SP - 6391
EP - 6398
JO - ACS Sustainable Chemistry and Engineering
JF - ACS Sustainable Chemistry and Engineering
SN - 2168-0485
IS - 12
ER -