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 - 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 - https://www.scopus.com/pages/publications/85122668826
U2 - 10.1021/acs.nanolett.1c04247
DO - 10.1021/acs.nanolett.1c04247
M3 - 文章
C2 - 34965149
AN - SCOPUS:85122668826
SN - 1530-6984
VL - 22
SP - 441
EP - 447
JO - Nano Letters
JF - Nano Letters
IS - 1
ER -