气候变化领域集成服务门户(CCPortal): Electrochemical implications of modulating the solvation shell around redox active organic species in aqueous organic redox flow batteries

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DOI	10.1073/pnas.2105889118
	Electrochemical implications of modulating the solvation shell around redox active organic species in aqueous organic redox flow batteries
	Sharma K.; Sankarasubramanian S.; Parrondo J.; Ramani V.
发表日期	2021
ISSN	0027-8424
卷号	118 期号:34
英文摘要	Organic and organometallic reactants in aqueous electrolytes, being composed of earth-abundant elements, are promising redox active candidates for cost-effective organic redox flow batteries (ORFBs). Various compounds of ferrocene and methyl viologen have been examined as promising redox actives for this application. Herein, we examined the influence of the electrolyte pH and the salt anion on model redox active organic cations, bis((3-trimethylammonio) propyl)- ferrocene dichloride (BTMAP-Fc) and bis(3trimethylammonio) propyl viologen tetrachloride (BTMAP-Vi), which have exhibited excellent cycling stability and capacity retention at ≥1.00 M concentration [E. S. Beh, et al. ACS Energy Lett. 2, 639–644 (2017)]. We examined the solvation shell around BTMAP-Fc and BTMAP-Vi at acidic and neutral pH with SO42-, Cl-, and CH3SO3- counterions and elucidated their impact on cation diffusion coefficient, first electron transfer rate constant, and thereby the electrochemical Thiele modulus. The electrochemical Thiele modulus was found to be exponentially correlated with the solvent reorganizational energy (λ) in both neutral and acidic pH. Thus, λ is proposed as a universal descriptor and selection criteria for organic redox flow battery electrolyte compositions. In the specific case of the BTMAP-Fc/BTMAP-Vi ORFB, low pH electrolytes with methanesulfonate or chloride counterions were identified as offering the best balance of transport and kinetic requirements. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	Effectiveness factor; Marcus–Hush theory; Organic active species; Redox flow battery; Thiele modulus
语种	英语
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/238419
作者单位	Center for Solar Energy and Energy Storage, Washington University in St. Louis, St. Louis, MO 63130, United States; Department of Energy, Environmental & Chemical Engineering, Washington University in St. Louis, St. Louis, MO 63130, United States; McKelvey School of Engineering, Washington University in St. Louis, St. Louis, MO 63130, United States
推荐引用方式 GB/T 7714	Sharma K.,Sankarasubramanian S.,Parrondo J.,et al. Electrochemical implications of modulating the solvation shell around redox active organic species in aqueous organic redox flow batteries[J],2021,118(34).
APA	Sharma K.,Sankarasubramanian S.,Parrondo J.,&Ramani V..(2021).Electrochemical implications of modulating the solvation shell around redox active organic species in aqueous organic redox flow batteries.Proceedings of the National Academy of Sciences of the United States of America,118(34).
MLA	Sharma K.,et al."Electrochemical implications of modulating the solvation shell around redox active organic species in aqueous organic redox flow batteries".Proceedings of the National Academy of Sciences of the United States of America 118.34(2021).