Hyung-Seok Lim1,Sujong Chae1,Litao Yan1,Guosheng Li1,Ruozhu Feng1,Yongsoon Shin1,Zimin Nie1,Bhuvaneswari Sivakumar1,Xin Zhang1,Yangang Liang1,David Bazak1,Vaithiyalingam Shutthanandan1,Vijayakumar Murugesan1,Soowhan Kim1,Wei Wang1
Pacific Northwest National Laboratory1
Hyung-Seok Lim1,Sujong Chae1,Litao Yan1,Guosheng Li1,Ruozhu Feng1,Yongsoon Shin1,Zimin Nie1,Bhuvaneswari Sivakumar1,Xin Zhang1,Yangang Liang1,David Bazak1,Vaithiyalingam Shutthanandan1,Vijayakumar Murugesan1,Soowhan Kim1,Wei Wang1
Pacific Northwest National Laboratory1
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 <sup>1</sup>H 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.