TY - JOUR
T1 - Carbon-Nanotube-Encapsulated-Sulfur Cathodes for Lithium-Sulfur Batteries
T2 - Integrated Computational Design and Experimental Validation
AU - Lin, Yuxiao
AU - Ticey, Jeremy
AU - Oleshko, Vladimir
AU - Zhu, Yujie
AU - Zhao, Xinsheng
AU - Wang, Chunsheng
AU - Cumings, John
AU - Qi, Yue
N1 - Funding Information:
We acknowledge the initial support from the Nanostructures for Electrical Energy Storage (NEES), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under Award number DESC0001160.
Publisher Copyright:
© 2021 American Chemical Society.
PY - 2022/1/12
Y1 - 2022/1/12
N2 - To mitigate lithium-polysulfides (Li-PSs) shuttle in lithium-sulfur batteries (LiSBs), a unique carbon-nanotube-encapsulated-sulfur (S@CNT) cathode material with optimum open-ring sizes (ORSs) on the CNT walls were designed using an integrated computational approach followed by experimental validation. By calculating the transport barrier of Li+ ion through ORSs on the CNT walls and comparing the molecular size of solvents and Li-PSs with ORSs, optimum open-rings with 16-30 surrounding carbon atoms were predicted to selectively allow transportation of Li+ ion and evaporated sulfur while blocking both Li-PS and solvent molecules. A CNT oxidation process was proposed and simulated to generate these ORSs, and the results indicated that the optimum ORSs can be achieved by narrowly controlling the oxidation parameters. Subsequently, S@CNT cathodes were experimentally synthesized, confirming that optimum ORSs were generated in CNT oxidized at 475 K and exhibited more stable cycling behavior.
AB - To mitigate lithium-polysulfides (Li-PSs) shuttle in lithium-sulfur batteries (LiSBs), a unique carbon-nanotube-encapsulated-sulfur (S@CNT) cathode material with optimum open-ring sizes (ORSs) on the CNT walls were designed using an integrated computational approach followed by experimental validation. By calculating the transport barrier of Li+ ion through ORSs on the CNT walls and comparing the molecular size of solvents and Li-PSs with ORSs, optimum open-rings with 16-30 surrounding carbon atoms were predicted to selectively allow transportation of Li+ ion and evaporated sulfur while blocking both Li-PS and solvent molecules. A CNT oxidation process was proposed and simulated to generate these ORSs, and the results indicated that the optimum ORSs can be achieved by narrowly controlling the oxidation parameters. Subsequently, S@CNT cathodes were experimentally synthesized, confirming that optimum ORSs were generated in CNT oxidized at 475 K and exhibited more stable cycling behavior.
KW - carbon-nanotube-encapsulated-sulfur cathodes
KW - integrated computational design
KW - lithium polysulfides shuttle
KW - optimum open-ring size
KW - theoretical criteria for the synthesis
UR - http://www.scopus.com/inward/record.url?scp=85122668826&partnerID=8YFLogxK
UR - https://www.mendeley.com/catalogue/44e447f1-a260-3f01-9a0b-c6c124ffa97a/
U2 - 10.1021/acs.nanolett.1c04247
DO - 10.1021/acs.nanolett.1c04247
M3 - Article
C2 - 34965149
AN - SCOPUS:85122668826
SN - 1530-6984
VL - 22
SP - 441
EP - 447
JO - Nano Letters
JF - Nano Letters
IS - 1
ER -