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Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries

Author

Listed:
  • Zhixuan Wei

    (Jilin University
    Oregon State University)

  • Woochul Shin

    (Oregon State University)

  • Heng Jiang

    (Oregon State University)

  • Xianyong Wu

    (Oregon State University)

  • William F. Stickle

    (Hewlett-Packard Co)

  • Gang Chen

    (Jilin University)

  • Jun Lu

    (Argonne National Laboratory)

  • P. Alex Greaney

    (University of California)

  • Fei Du

    (Jilin University)

  • Xiulei Ji

    (Oregon State University)

Abstract

The interactions between 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. Here 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.

Suggested Citation

  • Zhixuan Wei & Woochul Shin & Heng Jiang & Xianyong Wu & William F. Stickle & Gang Chen & Jun Lu & P. Alex Greaney & Fei Du & Xiulei Ji, 2019. "Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-11218-5
    DOI: 10.1038/s41467-019-11218-5
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    Cited by:

    1. Songshan Bi & Shuai Wang & Fang Yue & Zhiwei Tie & Zhiqiang Niu, 2021. "A rechargeable aqueous manganese-ion battery based on intercalation chemistry," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    2. Chang-Wei Bai & Lian-Lian Liu & Jie-Jie Chen & Fei Chen & Zhi-Quan Zhang & Yi-Jiao Sun & Xin-Jia Chen & Qi Yang & Han-Qing Yu, 2024. "Circumventing bottlenecks in H2O2 photosynthesis over carbon nitride with iodine redox chemistry and electric field effects," Nature Communications, Nature, vol. 15(1), pages 1-16, December.

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