Volume 9 Issue 4
Apr.  2024
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Article Navigation >  Green Energy&Environment  > 2024  >  9(4): 713-722
Zhifeng Huang, Rolf Hempelmann, Yiqiong Zhang, Li Tao, Ruiyong Chen. Pairing nitroxyl radical and phenazine with electron-withdrawing/-donating substituents in “water-in-ionic liquid” for high-voltage aqueous redox flow batteries. Green Energy&Environment, 2024, 9(4): 713-722. doi: 10.1016/j.gee.2022.09.005
Citation: Zhifeng Huang, Rolf Hempelmann, Yiqiong Zhang, Li Tao, Ruiyong Chen. Pairing nitroxyl radical and phenazine with electron-withdrawing/-donating substituents in “water-in-ionic liquid” for high-voltage aqueous redox flow batteries. Green Energy&Environment, 2024, 9(4): 713-722. doi: 10.1016/j.gee.2022.09.005
shu

Pairing nitroxyl radical and phenazine with electron-withdrawing/-donating substituents in “water-in-ionic liquid” for high-voltage aqueous redox flow batteries

doi: 10.1016/j.gee.2022.09.005

  • a. Transfercenter Sustainable Electrochemistry, Saarland University and KIST Europe, 66125, Saarbrücken, Germany;

  • b. State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University, Changsha, 410082, Hunan, China;

  • c. College of Materials Science and Engineering Changsha University of Science and Technology, Changsha, 410114, Hunan, China;

  • d. Materials Innovation Factory, Department of Chemistry, University of Liverpool, Liverpool, L69 7ZD, United Kingdom

Funds:

Z.H. acknowledges the support from China Postdoctoral Science Foundation (Grant No. 2021M690960) and China CSC abroad studying fellowship. R.C. thanks the KIST Europe basic research funding “new electrolytes for redox flow batteries” and the partial financial support from the CMBlu Energy AG. Y.Z. thanks to the support received from the National Natural Science Foundation of China (Grant No. 22002009) and the Natural Science Foundation of Hunan Province (Grant No. 2021JJ40565).

  • Received date 14 July 2022, Accepted date 13 September 2022, RevRecd date 06 September 2022, Publish date 17 September 2022,
    Abstract
  • Aqueous redox-active organic materials-base electrolytes are sustainable alternatives to vanadium-based electrolyte for redox flow batteries (RFBs) due to the advantages of high ionic conductivity, environmentally benign, safety and low cost. However, the underexplored redox properties of organic materials and the narrow thermodynamic electrolysis window of water (1.23 V) hinder their wide applications. Therefore, seeking suitable organic redox couples and aqueous electrolytes with a high output voltage is highly suggested for advancing the aqueous organic RFBs. In this work, the functionalized phenazine and nitroxyl radical with electron-donating and electron-withdrawing group exhibit redox potential of -0.88 V and 0.78 V vs. Ag, respectively, in “water-in-ionic liquid” supporting electrolytes. Raman spectra reveal that the activity of water is largely suppressed in “water-in-ionic liquid” due to the enhanced hydrogen bond interactions between ionic liquid and water, enabling an electrochemical stability window above 3 V. “Water-in-ionic liquid” supporting electrolytes help to shift redox potential of nitroxyl radical and enable the redox activity of functionalized phenazine. The assembled aqueous RFB allows a theoretical cell voltage of 1.66 V and shows a practical discharge voltage of 1.5 V in the “water-in-ionic liquid” electrolytes. Meanwhile, capacity retention of 99.91% per cycle is achieved over 500 charge/discharge cycles. A power density of 112 mW cm-2 is obtained at a current density of 30 mA cm-2. This work highlights the importance of rationally combining supporting electrolytes and organic molecules to achieve high-voltage aqueous RFBs.

     

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