Symmetry-breaking design of an organic iron complex catholyte for a long cyclability aqueous organic redox flow battery

Xiang Li, Peiyuan Gao, Yun-Yu Lai, J. David Bazak, Aaron Hollas, Heng-Yi Lin, Vijayakumar Murugesan, Shuyuan Zhang, Chung-Fu Cheng, Wei-Yao Tung, Yueh-Ting Lai, Ruozhu Feng, Jin Wang, Chien-Lung Wang, Wei Wang () and Yu Zhu ()
Additional contact information
Xiang Li: The University of Akron
Peiyuan Gao: Pacific Northwest National Laboratory
Yun-Yu Lai: The University of Akron
J. David Bazak: Pacific Northwest National Laboratory
Aaron Hollas: Pacific Northwest National Laboratory
Heng-Yi Lin: The University of Akron
Vijayakumar Murugesan: Pacific Northwest National Laboratory
Shuyuan Zhang: The University of Akron
Chung-Fu Cheng: The University of Akron
Wei-Yao Tung: The University of Akron
Yueh-Ting Lai: The University of Akron
Ruozhu Feng: Pacific Northwest National Laboratory
Jin Wang: The University of Akron
Chien-Lung Wang: National Yang Ming Chiao Tung University
Wei Wang: Pacific Northwest National Laboratory
Yu Zhu: The University of Akron

Nature Energy, 2021, vol. 6, issue 9, 873-881

Abstract: Abstract The limited availability of a high-performance catholyte has hindered the development of aqueous organic redox flow batteries (AORFB) for large-scale energy storage. Here we report a symmetry-breaking design of iron complexes with 2,2′-bipyridine-4,4′-dicarboxylic (Dcbpy) acid and cyanide ligands. By introducing two ligands to the metal centre, the complex compounds (M4[FeII(Dcbpy)2(CN)2], M = Na, K) exhibited up to a 4.2 times higher solubility (1.22 M) than that of M4[FeII(Dcbpy)3] and a 50% increase in potential compared with that of ferrocyanide. The AORFBs with 0.1 M Na4[FeII(Dcbpy)2(CN)2] as the catholyte were demonstrated for 6,000 cycles with a capacity fading rate of 0.00158% per cycle (0.217% per day). Even at a concentration near the solubility limit (1 M Na4[FeII(Dcbpy)2(CN)2]), the flow battery exhibited a capacity fading rate of 0.008% per cycle (0.25% per day) in the first 400 cycles. The AORFB cell with a nearly 1:1 catholyte:anolyte electron ratio achieved a cell voltage of 1.2 V and an energy density of 12.5 Wh l–1.

Date: 2021
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DOI: 10.1038/s41560-021-00879-6

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