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Title: 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:
 [1];  [2];  [2];  [2];  [3];  [4]; ORCiD logo [5]; ORCiD logo [6];  [4]; ORCiD logo [2]
  1. Jilin Univ., Changchun (China); Oregon State Univ., Corvallis, OR (United States)
  2. Oregon State Univ., Corvallis, OR (United States)
  3. Hewlett-Packard Co., Corvallis, OR (United States)
  4. Jilin Univ., Changchun (China)
  5. Argonne National Lab. (ANL), Lemont, IL (United States)
  6. Univ. of California, Riverside, CA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (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. 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, and Ji, Xiulei. Fri . "Reversible intercalation of methyl viologen as a dicationic charge carrier in aqueous batteries". United States. doi: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 = {2019},
month = {7}
}

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    Works referencing / citing this record:

    Sodium-Ion Batteries
    journal, May 2012

    • Slater, Michael D.; Kim, Donghan; Lee, Eungje
    • Advanced Functional Materials, Vol. 23, Issue 8, p. 947-958
    • DOI: 10.1002/adfm.201200691

    Sodium Storage Behavior in Natural Graphite using Ether-based Electrolyte Systems
    journal, November 2014

    • Kim, Haegyeom; Hong, Jihyun; Park, Young-Uk
    • Advanced Functional Materials, Vol. 25, Issue 4
    • DOI: 10.1002/adfm.201402984

    Layered P2-Type K 0.65 Fe 0.5 Mn 0.5 O 2 Microspheres as Superior Cathode for High-Energy Potassium-Ion Batteries
    journal, May 2018

    • Deng, Tao; Fan, Xiulin; Chen, Ji
    • Advanced Functional Materials, Vol. 28, Issue 28
    • DOI: 10.1002/adfm.201800219

    Rechargeable Aqueous Zinc-Ion Battery Based on Porous Framework Zinc Pyrovanadate Intercalation Cathode
    journal, December 2017


    An Aqueous Ca-Ion Battery
    journal, October 2017

    • Gheytani, Saman; Liang, Yanliang; Wu, Feilong
    • Advanced Science, Vol. 4, Issue 12
    • DOI: 10.1002/advs.201700465

    Tailored Aromatic Carbonyl Derivative Polyimides for High-Power and Long-Cycle Sodium-Organic Batteries
    journal, December 2013

    • Wang, Heng-guo; Yuan, Shuang; Ma, De-long
    • Advanced Energy Materials, Vol. 4, Issue 7
    • DOI: 10.1002/aenm.201301651

    A Novel Aluminum-Graphite Dual-Ion Battery
    journal, March 2016

    • Zhang, Xiaolong; Tang, Yongbing; Zhang, Fan
    • Advanced Energy Materials, Vol. 6, Issue 11
    • DOI: 10.1002/aenm.201502588

    Toward a High-Performance All-Plastic Full Battery with a'Single Organic Polymer as Both Cathode and Anode
    journal, April 2018

    • Xie, Jian; Wang, Zilong; Xu, Zhichuan J.
    • Advanced Energy Materials, Vol. 8, Issue 21
    • DOI: 10.1002/aenm.201703509

    Reversible S 0 /MgS x Redox Chemistry in a MgTFSI 2 /MgCl 2 /DME Electrolyte for Rechargeable Mg/S Batteries
    journal, September 2017


    The Emerging Chemistry of Sodium Ion Batteries for Electrochemical Energy Storage
    journal, February 2015

    • Kundu, Dipan; Talaie, Elahe; Duffort, Victor
    • Angewandte Chemie International Edition, Vol. 54, Issue 11
    • DOI: 10.1002/anie.201410376

    A Sulfur Heterocyclic Quinone Cathode and a Multifunctional Binder for a High-Performance Rechargeable Lithium-Ion Battery
    journal, April 2016

    • Ma, Ting; Zhao, Qing; Wang, Jianbin
    • Angewandte Chemie International Edition, Vol. 55, Issue 22
    • DOI: 10.1002/anie.201601119

    Hydronium-Ion Batteries with Perylenetetracarboxylic Dianhydride Crystals as an Electrode
    journal, February 2017

    • Wang, Xingfeng; Bommier, Clement; Jian, Zelang
    • Angewandte Chemie International Edition, Vol. 56, Issue 11
    • DOI: 10.1002/anie.201700148

    An Insoluble Benzoquinone-Based Organic Cathode for Use in Rechargeable Lithium-Ion Batteries
    journal, August 2017

    • Luo, Zhiqiang; Liu, Luojia; Zhao, Qing
    • Angewandte Chemie International Edition, Vol. 56, Issue 41
    • DOI: 10.1002/anie.201706604

    Rocking-Chair Ammonium-Ion Battery: A Highly Reversible Aqueous Energy Storage System
    journal, September 2017

    • Wu, Xianyong; Qi, Yitong; Hong, Jessica J.
    • Angewandte Chemie International Edition, Vol. 56, Issue 42
    • DOI: 10.1002/anie.201707473

    Organic Thiocarboxylate Electrodes for a Room-Temperature Sodium-Ion Battery Delivering an Ultrahigh Capacity
    journal, November 2017

    • Zhao, Hongyang; Wang, Jianwei; Zheng, Yuheng
    • Angewandte Chemie International Edition, Vol. 56, Issue 48
    • DOI: 10.1002/anie.201708960

    Synthesis and Exploration of Ladder-Structured Large Aromatic Dianhydrides as Organic Cathodes for Rechargeable Lithium-Ion Batteries
    journal, March 2017

    • Xie, Jian; Chen, Wangqiao; Wang, Zilong
    • Chemistry - An Asian Journal, Vol. 12, Issue 8
    • DOI: 10.1002/asia.201700070

    Graphene Scroll-Coated α-MnO 2 Nanowires as High-Performance Cathode Materials for Aqueous Zn-Ion Battery
    journal, February 2018


    Sodium Peroxide Dihydrate or Sodium Superoxide: The Importance of the Cell Configuration for Sodium-Oxygen Batteries
    journal, May 2017


    Antibacterial activity of polymeric substrate with surface grafted viologen moieties
    journal, February 2005


    High-rate and long-life VS2 cathodes for hybrid magnesium-based battery
    journal, May 2018


    Hybrid Aqueous/Non-aqueous Electrolyte for Safe and High-Energy Li-Ion Batteries
    journal, May 2018


    Organic electrode for non-aqueous potassium-ion batteries
    journal, November 2015


    Nanostructured Conjugated Polymers: Toward High-Performance Organic Electrodes for Rechargeable Batteries
    journal, August 2017


    Asymmetric K/Li-Ion Battery Based on Intercalation Selectivity
    journal, November 2017


    Abnormal Excess Capacity of Conjugated Dicarboxylates in Lithium-Ion Batteries
    journal, October 2014

    • Lee, Hyun Ho; Park, Yuwon; Shin, Kyoung-Hee
    • ACS Applied Materials & Interfaces, Vol. 6, Issue 21
    • DOI: 10.1021/am505090p

    How Ions Affect the Structure of Water
    journal, October 2002

    • Hribar, Barbara; Southall, Noel T.; Vlachy, Vojko
    • Journal of the American Chemical Society, Vol. 124, Issue 41
    • DOI: 10.1021/ja026014h

    Phosphorus-Based Alloy Materials for Advanced Potassium-Ion Battery Anode
    journal, February 2017

    • Zhang, Wenchao; Mao, Jianfeng; Li, Sean
    • Journal of the American Chemical Society, Vol. 139, Issue 9
    • DOI: 10.1021/jacs.6b12185

    Mg-Ion Battery Electrode: An Organic Solid’s Herringbone Structure Squeezed upon Mg-Ion Insertion
    journal, September 2017

    • Rodríguez-Pérez, Ismael A.; Yuan, Yifei; Bommier, Clement
    • Journal of the American Chemical Society, Vol. 139, Issue 37
    • DOI: 10.1021/jacs.7b06313

    Molecular Organization of LB Multilayers of Phospholipid and Mixed Phospholipid/Viologen By FTIR Spectroscopy
    journal, June 2002

    • Lozano, P.; Fernández, A. J.; Ruiz, J. J.
    • The Journal of Physical Chemistry B, Vol. 106, Issue 25
    • DOI: 10.1021/jp0144505

    A class of liquid anode for rechargeable batteries with ultralong cycle life
    journal, March 2017

    • Yu, Juezhi; Hu, Yong-Sheng; Pan, Feng
    • Nature Communications, Vol. 8, Issue 1
    • DOI: 10.1038/ncomms14629

    Biologically inspired pteridine redox centres for rechargeable batteries
    journal, October 2014

    • Hong, Jihyun; Lee, Minah; Lee, Byungju
    • Nature Communications, Vol. 5, Issue 1
    • DOI: 10.1038/ncomms6335

    Reviving the lithium metal anode for high-energy batteries
    journal, March 2017

    • Lin, Dingchang; Liu, Yayuan; Cui, Yi
    • Nature Nanotechnology, Vol. 12, Issue 3
    • DOI: 10.1038/nnano.2017.16

    Highly reversible zinc metal anode for aqueous batteries
    journal, April 2018


    Environmentally-friendly aqueous Li (or Na)-ion battery with fast electrode kinetics and super-long life
    journal, January 2016


    High-capacity aqueous zinc batteries using sustainable quinone electrodes
    journal, March 2018