Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries
Abstract
The interactions among charge carriers and electrode structures represent one of the most important considerations in the search for new energy storage devices. Currently, ionic bonding dominates the battery chemistry. In this work we report the reversible insertion of a large molecular dication, methyl viologen, into the crystal structure of an aromatic solid electrode, 3,4,9,10-perylenetetracarboxylic dianhydride. This is the largest insertion charge carrier when non-solvated ever reported for batteries; surprisingly, the kinetic properties of the (de) insertion of methyl viologen are excellent with 60% of capacity retained when the current rate is increased from 100 mA g-1 to 2000 mA g-1. Characterization reveals that the insertion of methyl viologen causes phase transformation of the organic host, and embodies guest-host chemical bonding. First-principles density functional theory calculations suggest strong guest-host interaction beyond the pure ionic bonding, where a large extent of covalency may exist. This study extends the boundary of battery chemistry to large molecular ions as charge carriers and also highlights the electrochemical assembly of a supramolecular system.
- Authors:
-
[5];
[6];
[2]
- Jilin Univ., Changchun (China); Oregon State Univ., Corvallis, OR (United States)
- Oregon State Univ., Corvallis, OR (United States)
- Hewlett-Packard Co., Corvallis, OR (United States)
- Jilin Univ., Changchun (China)
- Argonne National Lab. (ANL), Lemont, IL (United States)
- Univ. of California, Riverside, CA (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF); China Scholarship Council (CSC)
- OSTI Identifier:
- 1558087
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Wei, Zhixuan, Shin, Woochul, Jiang, Heng, Wu, Xianyong, Stickle, William F., Chen, Gang, Lu, Jun, Alex Greaney, P., Du, Fei, and Ji, Xiulei. Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries. United States: N. p., 2019.
Web. doi:10.1038/s41467-019-11218-5.
Wei, Zhixuan, Shin, Woochul, Jiang, Heng, Wu, Xianyong, Stickle, William F., Chen, Gang, Lu, Jun, Alex Greaney, P., Du, Fei, & Ji, Xiulei. Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries. United States. https://doi.org/10.1038/s41467-019-11218-5
Wei, Zhixuan, Shin, Woochul, Jiang, Heng, Wu, Xianyong, Stickle, William F., Chen, Gang, Lu, Jun, Alex Greaney, P., Du, Fei, and Ji, Xiulei. Fri .
"Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries". United States. https://doi.org/10.1038/s41467-019-11218-5. https://www.osti.gov/servlets/purl/1558087.
@article{osti_1558087,
title = {Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries},
author = {Wei, Zhixuan and Shin, Woochul and Jiang, Heng and Wu, Xianyong and Stickle, William F. and Chen, Gang and Lu, Jun and Alex Greaney, P. and Du, Fei and Ji, Xiulei},
abstractNote = {The interactions among charge carriers and electrode structures represent one of the most important considerations in the search for new energy storage devices. Currently, ionic bonding dominates the battery chemistry. In this work we report the reversible insertion of a large molecular dication, methyl viologen, into the crystal structure of an aromatic solid electrode, 3,4,9,10-perylenetetracarboxylic dianhydride. This is the largest insertion charge carrier when non-solvated ever reported for batteries; surprisingly, the kinetic properties of the (de) insertion of methyl viologen are excellent with 60% of capacity retained when the current rate is increased from 100 mA g-1 to 2000 mA g-1. Characterization reveals that the insertion of methyl viologen causes phase transformation of the organic host, and embodies guest-host chemical bonding. First-principles density functional theory calculations suggest strong guest-host interaction beyond the pure ionic bonding, where a large extent of covalency may exist. This study extends the boundary of battery chemistry to large molecular ions as charge carriers and also highlights the electrochemical assembly of a supramolecular system.},
doi = {10.1038/s41467-019-11218-5},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Fri Jul 19 00:00:00 EDT 2019},
month = {Fri Jul 19 00:00:00 EDT 2019}
}
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Works referencing / citing this record:
A paradigm of storage batteries
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