Phosphonate-based iron complex for a cost-effective and long cycling aqueous iron redox flow battery

Gabriel S. Nambafu, Aaron M. Hollas, Shuyuan Zhang, Peter S. Rice, Daria Boglaienko, John L. Fulton, Miller Li, Qian Huang, Yu Zhu, David M. Reed, Vincent L. Sprenkle and Guosheng Li ()
Additional contact information
Gabriel S. Nambafu: Energy & Environment Directorate, Pacific Northwest National Laboratory
Aaron M. Hollas: Energy & Environment Directorate, Pacific Northwest National Laboratory
Shuyuan Zhang: School of Polymer Science and Polymer Engineering, The University of Akron
Peter S. Rice: Physical & Computational Science, Directorate, Pacific Northwest National Laboratory
Daria Boglaienko: Energy & Environment Directorate, Pacific Northwest National Laboratory
John L. Fulton: Physical & Computational Science, Directorate, Pacific Northwest National Laboratory
Miller Li: Energy & Environment Directorate, Pacific Northwest National Laboratory
Qian Huang: Energy & Environment Directorate, Pacific Northwest National Laboratory
Yu Zhu: School of Polymer Science and Polymer Engineering, The University of Akron
David M. Reed: Energy & Environment Directorate, Pacific Northwest National Laboratory
Vincent L. Sprenkle: Energy & Environment Directorate, Pacific Northwest National Laboratory
Guosheng Li: Energy & Environment Directorate, Pacific Northwest National Laboratory

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract A promising metal-organic complex, iron (Fe)-NTMPA2, consisting of Fe(III) chloride and nitrilotri-(methylphosphonic acid) (NTMPA), is designed for use in aqueous iron redox flow batteries. A full-cell testing, where a concentrated Fe-NTMPA2 anolyte (0.67 M) is paired with a Fe-CN catholyte, demonstrates exceptional cycling stability over 1000 charge/discharge cycles, and noteworthy performances, including 96% capacity utilization, a minimal capacity fade rate of 0.0013% per cycle (1.3% over 1,000 cycles), high Coulombic efficiency and energy efficiency near 100% and 87%, respectively, all achieved under a current density of 20 mA·cm-². Furthermore, density functional theory unveils two potential coordination structures for Fe-NTMPA2 complexes, improving the understanding between the ligand coordination environment and electron transfer kinetics. When paired with a high redox potential Fe-Dcbpy/CN catholyte, 2,2′-bipyridine-4,4′-dicarboxylic (Dcbpy) acid and cyanide (CN) ligands, Fe-NTMPA2 demonstrates a notably elevated cell voltage of 1 V, enabling a practical energy density of up to 9 Wh/L.

Date: 2024
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DOI: 10.1038/s41467-024-45862-3

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