Journal
CHEM
Volume 3, Issue 6, Pages 961-978Publisher
CELL PRESS
DOI: 10.1016/j.chempr.2017.11.001
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Funding
- Utah State University
- Utah Science Technology and Research Initiative
- USU Presidential Doctoral Research Fellowship program
- China CSC Study Abroad program
- Utah Energy Triangle Student Award
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Aqueous organic redox flow batteries (AORFBs) are highly attractive for large-scale energy storage because redox-active organic molecules are synthetically tunable, sustainable, and potentially low cost. Here, we show that rational molecular engineering yielded a series of two-electron storage viologen molecules as anolyte materials for AORFBs. In neutral NaCl solutions, these viologen anolytes have a theoretical capacity of up to 96.5 Ah/L in H2O and exhibit a reduction potential as low as -0.78 V versus normal hydrogen electrode. The neutral aqueous flow batteries with two two-electron storage viologen molecules delivered a cell voltage of up to 1.38 V and outstanding battery performance, including a power density of up to 130 mW/cm(2), capacity retention of up to 99.99% per cycle, and energy efficiency of up to 65% at 60 mA/cm(2). Density functional theory calculations revealed that the 1e(-) and 2e(-) reduced redox states of these molecules were stabilized by the high charge delocalization of their frontier SOMO or HOMO.
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