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Redox flow batteries are considered a promising technology for grid energy storage. However, capacity decay caused by crossover of active materials is a universal challenge for many flow battery systems, which are based on various chemistries. In this work, we demonstrate a new gel polymer interface (GPI) consisting of crosslinked polyethyleneimine with a large amount of amino and carboxylic acid groups introduced between the positive electrode and the membrane. The GPI functions as a key component to prevent vanadium ions from crossing the membrane, thus supporting stable long-term cycling. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) measurements were conducted to investigate the effect of GPI on the electrochemical properties of graphitic carbon electrodes (GCFs) and redox reaction of catholyte. Results from inductively coupled plasma mass spectrometry (ICP-MS), Fourier-transform infrared (FTIR) spectroscopy, and energy-dispersive X-ray (EDX) spectroscopy proved that the GPI is effective in maintaining the concentration of vanadium species in their respective half-cells, resulting in improved cycling stability because of it prevents active species from crossing the membrane and stabilizes the oxidation states of active species. X-ray photoelectron spectroscopy (XPS) and ¹H nuclear magnetic resonance (NMR) spectra demonstrated that the cross-linked GPI is chemically stable for 100 cycles without dissolution of polymers and swelling in the strong acidic electrolytes.

Co-Author(s): Sujong Chae (Pacific Northwest National Laboratory), Litao Yan (Pacific Northwest National Laboratory), Guosheng Li (Pacific Northwest National Laboratory), Ruozhu Feng (Pacific Northwest National Laboratory), Yongsoon Shin (Pacific Northwest National Laboratory), Zimin Nie (Pacific Northwest National Laboratory), Bhuvaneswari Sivakumar (Pacific Northwest National Laboratory), Xin Zhang (Pacific Northwest National Laboratory), Yangang Liang (Pacific Northwest National Laboratory), David Bazak (Pacific Northwest National Laboratory), Vaithiyalingam Shutthanandan (Pacific Northwest National Laboratory), Vijayakumar Murugesan (Pacific Northwest National Laboratory), Soowhan Kim (Pacific Northwest National Laboratory), Wei Wang (Pacific Northwest National Laboratory)

Hyung-Seok Lim

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