Electrochemical analysis of charge mediator product composition through transient model and experimental validation

Daniel Moreno; Jesse Thompson; Ayokunle Omosebi; James Landon; Kunlei Liu

doi:10.1007/s10800-022-01727-5

Electrochemical analysis of charge mediator product composition through transient model and experimental validation

Daniel Moreno, Jesse Thompson, Ayokunle Omosebi, James Landon, Kunlei Liu

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

1 Scopus citations

Abstract

Charge carriers have been studied for use in applications such as fuel cells, redox flow batteries, and electrochemical CO₂ reactors for conversion to value-added products. Here, transient-based equilibrium models are developed for two well-known charge carriers: methyl viologen (MV) and ethyl viologen (EV). The models are simulated using Butler-Volmer kinetics until steady-state is reached. EV is favored over MV due to lower dimerization, and enabling over 2 × production of reduced EV⁺ over MV⁺. MV and EV products do not appear to significantly change, except only under sufficiently acidic conditions (pH < 4). Charge and energy input requirement are used to assess total system efficiency and potential for system scale-up via chronoamperometry. The charge and energy analysis performed with EV as the charge carrier reveals that optimal charging voltage is around − 0.8 to − 0.85 V vs. Ag/AgCl, which is above the minimum reduction voltage (around − 0.6 to − 0.7 V vs. Ag/AgCl) and suggest more favorable conditions for performing such charge carrier reductions. Graphical abstract: [Figure not available: see fulltext.]

Original language	English
Pages (from-to)	1573-1584
Number of pages	12
Journal	Journal of Applied Electrochemistry
Volume	52
Issue number	11
DOIs	https://doi.org/10.1007/s10800-022-01727-5
State	Published - Nov 2022

Bibliographical note

Funding Information:
The authors would like to thank the U.S. Department of Energy for primary financial support for this project (Grant No. DE-FE0031720). The authors would also like to thank Dr. Susan Odom (University of Kentucky) for providing additional insight and discussion on the charge carrier structures, and Dr. Chin Ng (University of Kentucky) for contributions to the modeling equations.

Funding Information:
The authors would like to thank the U.S. Department of Energy for primary financial support for this project (Grant No. DE-FE0031720). The authors would also like to thank Dr. Susan Odom (University of Kentucky) for providing additional insight and discussion on the charge carrier structures, and Dr. Chin Ng (University of Kentucky) for contributions to the modeling equations.

Publisher Copyright:
© 2022, The Author(s), under exclusive licence to Springer Nature B.V.

Keywords

Batch cell reactor
Charge carrier
Chronoamperometry
Cyclic voltammetry
Electrocatalysis
Modeling
Speciation
Viologen

ASJC Scopus subject areas

Chemical Engineering (all)
Electrochemistry
Materials Chemistry

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10.1007/s10800-022-01727-5

Cite this

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title = "Electrochemical analysis of charge mediator product composition through transient model and experimental validation",

abstract = "Charge carriers have been studied for use in applications such as fuel cells, redox flow batteries, and electrochemical CO2 reactors for conversion to value-added products. Here, transient-based equilibrium models are developed for two well-known charge carriers: methyl viologen (MV) and ethyl viologen (EV). The models are simulated using Butler-Volmer kinetics until steady-state is reached. EV is favored over MV due to lower dimerization, and enabling over 2 × production of reduced EV+ over MV+. MV and EV products do not appear to significantly change, except only under sufficiently acidic conditions (pH < 4). Charge and energy input requirement are used to assess total system efficiency and potential for system scale-up via chronoamperometry. The charge and energy analysis performed with EV as the charge carrier reveals that optimal charging voltage is around − 0.8 to − 0.85 V vs. Ag/AgCl, which is above the minimum reduction voltage (around − 0.6 to − 0.7 V vs. Ag/AgCl) and suggest more favorable conditions for performing such charge carrier reductions. Graphical abstract: [Figure not available: see fulltext.]",

keywords = "Batch cell reactor, Charge carrier, Chronoamperometry, Cyclic voltammetry, Electrocatalysis, Modeling, Speciation, Viologen",

author = "Daniel Moreno and Jesse Thompson and Ayokunle Omosebi and James Landon and Kunlei Liu",

note = "Funding Information: The authors would like to thank the U.S. Department of Energy for primary financial support for this project (Grant No. DE-FE0031720). The authors would also like to thank Dr. Susan Odom (University of Kentucky) for providing additional insight and discussion on the charge carrier structures, and Dr. Chin Ng (University of Kentucky) for contributions to the modeling equations. Funding Information: The authors would like to thank the U.S. Department of Energy for primary financial support for this project (Grant No. DE-FE0031720). The authors would also like to thank Dr. Susan Odom (University of Kentucky) for providing additional insight and discussion on the charge carrier structures, and Dr. Chin Ng (University of Kentucky) for contributions to the modeling equations. Publisher Copyright: {\textcopyright} 2022, The Author(s), under exclusive licence to Springer Nature B.V.",

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AU - Landon, James

AU - Liu, Kunlei

N1 - Funding Information: The authors would like to thank the U.S. Department of Energy for primary financial support for this project (Grant No. DE-FE0031720). The authors would also like to thank Dr. Susan Odom (University of Kentucky) for providing additional insight and discussion on the charge carrier structures, and Dr. Chin Ng (University of Kentucky) for contributions to the modeling equations. Funding Information: The authors would like to thank the U.S. Department of Energy for primary financial support for this project (Grant No. DE-FE0031720). The authors would also like to thank Dr. Susan Odom (University of Kentucky) for providing additional insight and discussion on the charge carrier structures, and Dr. Chin Ng (University of Kentucky) for contributions to the modeling equations. Publisher Copyright: © 2022, The Author(s), under exclusive licence to Springer Nature B.V.

PY - 2022/11

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N2 - Charge carriers have been studied for use in applications such as fuel cells, redox flow batteries, and electrochemical CO2 reactors for conversion to value-added products. Here, transient-based equilibrium models are developed for two well-known charge carriers: methyl viologen (MV) and ethyl viologen (EV). The models are simulated using Butler-Volmer kinetics until steady-state is reached. EV is favored over MV due to lower dimerization, and enabling over 2 × production of reduced EV+ over MV+. MV and EV products do not appear to significantly change, except only under sufficiently acidic conditions (pH < 4). Charge and energy input requirement are used to assess total system efficiency and potential for system scale-up via chronoamperometry. The charge and energy analysis performed with EV as the charge carrier reveals that optimal charging voltage is around − 0.8 to − 0.85 V vs. Ag/AgCl, which is above the minimum reduction voltage (around − 0.6 to − 0.7 V vs. Ag/AgCl) and suggest more favorable conditions for performing such charge carrier reductions. Graphical abstract: [Figure not available: see fulltext.]

AB - Charge carriers have been studied for use in applications such as fuel cells, redox flow batteries, and electrochemical CO2 reactors for conversion to value-added products. Here, transient-based equilibrium models are developed for two well-known charge carriers: methyl viologen (MV) and ethyl viologen (EV). The models are simulated using Butler-Volmer kinetics until steady-state is reached. EV is favored over MV due to lower dimerization, and enabling over 2 × production of reduced EV+ over MV+. MV and EV products do not appear to significantly change, except only under sufficiently acidic conditions (pH < 4). Charge and energy input requirement are used to assess total system efficiency and potential for system scale-up via chronoamperometry. The charge and energy analysis performed with EV as the charge carrier reveals that optimal charging voltage is around − 0.8 to − 0.85 V vs. Ag/AgCl, which is above the minimum reduction voltage (around − 0.6 to − 0.7 V vs. Ag/AgCl) and suggest more favorable conditions for performing such charge carrier reductions. Graphical abstract: [Figure not available: see fulltext.]

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Electrochemical analysis of charge mediator product composition through transient model and experimental validation

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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