Understanding capacity fade in organic redox-flow batteries by combining spectroscopy with statistical inference techniques

Modak, Sanat Vibhas; Shen, Wanggang; Singh, Siddhant; Herrera, Dylan; Oudeif, Fairooz; Goldsmith, Bryan R.; Huan, Xun; Kwabi, David G.

doi:10.1038/s41467-023-39257-z

Understanding capacity fade in organic redox-flow batteries by combining spectroscopy with statistical inference techniques

Journal Article · Fri Jun 16 00:00:00 EDT 2023 · Nature Communications

DOI:https://doi.org/10.1038/s41467-023-39257-z· OSTI ID:2423142

^[1]; ^[1]; Singh, Siddhant ^[1]; Herrera, Dylan ^[1]; Oudeif, Fairooz ^[1]; ^[1]; ^[1]; ^[1]

Univ. of Michigan, Ann Arbor, MI (United States)

Organic redox-active molecules are attractive as redox-flow battery (RFB) reactants because of their low anticipated costs and widely tunable properties. Unfortunately, many lab-scale flow cells experience rapid material degradation (from chemical and electrochemical decay mechanisms) and capacity fade during cycling (>0.1%/day) hindering their commercial deployment. In this work, we combine ultraviolet-visible spectrophotometry and statistical inference techniques to elucidate the Michael attack decay mechanism for 4,5-dihydroxy-1,3-benzenedisulfonic acid (BQDS), a once-promising positive electrolyte reactant for aqueous organic redox-flow batteries. We use Bayesian inference and multivariate curve resolution on the spectroscopic data to derive uncertainty-quantified reaction orders and rates for Michael attack, estimate the spectra of intermediate species and establish a quantitative connection between molecular decay and capacity fade. Our work illustrates the promise of using statistical inference to elucidate chemical and electrochemical mechanisms of capacity fade in organic redox-flow battery together with uncertainty quantification, in flow cell-based electrochemical systems.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Science Foundation (NSF)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2423142

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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