Proton-regulated alcohol oxidation for high-capacity ketone-based flow battery anolyte

Ruozhu Feng; Ying Chen; Xin Zhang; Benjamin J.G. Rousseau; Peiyuan Gao; Ping Chen; Sebastian T. Mergelsberg; Lirong Zhong; Aaron Hollas; Yangang Liang; Vijayakumar Murugesan; Qian Huang; Eric Walter; Sharon Hammes-Schiffer; Yuyan Shao; Wei Wang

doi:10.1016/j.joule.2023.06.013

Proton-regulated alcohol oxidation for high-capacity ketone-based flow battery anolyte

Ruozhu Feng
, Ying Chen
, Xin Zhang
, Benjamin J.G. Rousseau
, Peiyuan Gao
, Ping Chen
, Sebastian T. Mergelsberg
, Lirong Zhong
, Aaron Hollas
, Yangang Liang
, Vijayakumar Murugesan
, Qian Huang
, Eric Walter
, Sharon Hammes-Schiffer
, Yuyan Shao
, Wei Wang

Research output: Contribution to journal › Article › peer-review

19 Scopus citations

Abstract

Redox flow batteries have a unique architecture that potentially enables cost-effective long-duration energy storage to address the intermittency introduced by increased renewable integration for the decarbonization of the electric power sector. Targeted molecular engineering has demonstrated electrochemical reversibility in natively redox-inactive ketone molecules in aqueous electrolytes. However, the kinetics of fluorenone-based flow batteries continue to be limited by slow alcohol oxidation. We show how strategically designed proton regulators can accelerate alcohol oxidation and thus enhance battery kinetics. Fluorenone-based flow batteries with the organic additive β-cyclodextrin demonstrate enhanced rate capability, high capacity, and long cycling. This study opens a new avenue to improve the kinetics of aqueous organic flow batteries by modulating the reaction pathway with a homogeneous catalyst.

Original language	English (US)
Pages (from-to)	1609-1622
Number of pages	14
Journal	Joule
Volume	7
Issue number	7
DOIs	https://doi.org/10.1016/j.joule.2023.06.013
State	Published - Jul 19 2023
Externally published	Yes

All Science Journal Classification (ASJC) codes

General Energy

Keywords

H-bonding
H/D exchange
alcohol oxidation
comproportionation
fluorenone
homogeneous catalysis
in situ Electron paramagnetic resonance
proton coupled electron transfer
redox flow battery

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10.1016/j.joule.2023.06.013

Cite this

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title = "Proton-regulated alcohol oxidation for high-capacity ketone-based flow battery anolyte",

abstract = "Redox flow batteries have a unique architecture that potentially enables cost-effective long-duration energy storage to address the intermittency introduced by increased renewable integration for the decarbonization of the electric power sector. Targeted molecular engineering has demonstrated electrochemical reversibility in natively redox-inactive ketone molecules in aqueous electrolytes. However, the kinetics of fluorenone-based flow batteries continue to be limited by slow alcohol oxidation. We show how strategically designed proton regulators can accelerate alcohol oxidation and thus enhance battery kinetics. Fluorenone-based flow batteries with the organic additive β-cyclodextrin demonstrate enhanced rate capability, high capacity, and long cycling. This study opens a new avenue to improve the kinetics of aqueous organic flow batteries by modulating the reaction pathway with a homogeneous catalyst.",

keywords = "H-bonding, H/D exchange, alcohol oxidation, comproportionation, fluorenone, homogeneous catalysis, in situ Electron paramagnetic resonance, proton coupled electron transfer, redox flow battery",

author = "Ruozhu Feng and Ying Chen and Xin Zhang and Rousseau, \{Benjamin J.G.\} and Peiyuan Gao and Ping Chen and Mergelsberg, \{Sebastian T.\} and Lirong Zhong and Aaron Hollas and Yangang Liang and Vijayakumar Murugesan and Qian Huang and Eric Walter and Sharon Hammes-Schiffer and Yuyan Shao and Wei Wang",

note = "Publisher Copyright: {\textcopyright} 2023 Elsevier Inc.",

year = "2023",

month = jul,

day = "19",

doi = "10.1016/j.joule.2023.06.013",

language = "English (US)",

volume = "7",

pages = "1609--1622",

journal = "Joule",

issn = "2542-4351",

publisher = "Cell Press",

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TY - JOUR

T1 - Proton-regulated alcohol oxidation for high-capacity ketone-based flow battery anolyte

AU - Feng, Ruozhu

AU - Chen, Ying

AU - Zhang, Xin

AU - Rousseau, Benjamin J.G.

AU - Gao, Peiyuan

AU - Chen, Ping

AU - Mergelsberg, Sebastian T.

AU - Zhong, Lirong

AU - Hollas, Aaron

AU - Liang, Yangang

AU - Murugesan, Vijayakumar

AU - Huang, Qian

AU - Walter, Eric

AU - Hammes-Schiffer, Sharon

AU - Shao, Yuyan

AU - Wang, Wei

PY - 2023/7/19

Y1 - 2023/7/19

N2 - Redox flow batteries have a unique architecture that potentially enables cost-effective long-duration energy storage to address the intermittency introduced by increased renewable integration for the decarbonization of the electric power sector. Targeted molecular engineering has demonstrated electrochemical reversibility in natively redox-inactive ketone molecules in aqueous electrolytes. However, the kinetics of fluorenone-based flow batteries continue to be limited by slow alcohol oxidation. We show how strategically designed proton regulators can accelerate alcohol oxidation and thus enhance battery kinetics. Fluorenone-based flow batteries with the organic additive β-cyclodextrin demonstrate enhanced rate capability, high capacity, and long cycling. This study opens a new avenue to improve the kinetics of aqueous organic flow batteries by modulating the reaction pathway with a homogeneous catalyst.

AB - Redox flow batteries have a unique architecture that potentially enables cost-effective long-duration energy storage to address the intermittency introduced by increased renewable integration for the decarbonization of the electric power sector. Targeted molecular engineering has demonstrated electrochemical reversibility in natively redox-inactive ketone molecules in aqueous electrolytes. However, the kinetics of fluorenone-based flow batteries continue to be limited by slow alcohol oxidation. We show how strategically designed proton regulators can accelerate alcohol oxidation and thus enhance battery kinetics. Fluorenone-based flow batteries with the organic additive β-cyclodextrin demonstrate enhanced rate capability, high capacity, and long cycling. This study opens a new avenue to improve the kinetics of aqueous organic flow batteries by modulating the reaction pathway with a homogeneous catalyst.

KW - H-bonding

KW - H/D exchange

KW - alcohol oxidation

KW - comproportionation

KW - fluorenone

KW - homogeneous catalysis

KW - in situ Electron paramagnetic resonance

KW - proton coupled electron transfer

KW - redox flow battery

UR - https://www.scopus.com/pages/publications/85165066708

UR - https://www.scopus.com/pages/publications/85165066708#tab=citedBy

U2 - 10.1016/j.joule.2023.06.013

DO - 10.1016/j.joule.2023.06.013

M3 - Article

AN - SCOPUS:85165066708

SN - 2542-4351

VL - 7

SP - 1609

EP - 1622

JO - Joule

JF - Joule

IS - 7

ER -

Proton-regulated alcohol oxidation for high-capacity ketone-based flow battery anolyte

Abstract

All Science Journal Classification (ASJC) codes

Keywords

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