Effect of Polymer Variation in Cu-Polymer Composite Electrodes on Electrochemical CO2 Reduction

Heryn K. Wang; Chun Yat Sit; Richard T. Haasch; Paul J.A. Kenis; Andrew A. Gewirth

doi:10.1021/acsaem.4c03092

Effect of Polymer Variation in Cu-Polymer Composite Electrodes on Electrochemical CO₂ Reduction

Heryn K. Wang, Chun Yat Sit, Richard T. Haasch, Paul J.A. Kenis, Andrew A. Gewirth

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

Abstract

Cu-polyamine composite electrodes for the CO₂RR were prepared using three different amine-functionalized polymers: poly-l-lysine (PLL), poly-l-histidine (PLH), and poly-l-arginine (PLA). Of the composite electrodes, the Cu-PLL electrode demonstrated the highest selectivity for multicarbon (C₂₊) products, reaching an FE_C2+ of 74.3% at −0.98 V vs a reversible hydrogen electrode in a flow cell. In situ surface-enhanced Raman spectroscopy studies obtained from the composite electrodes show that a higher surface pH is achieved on the Cu-PLL electrode during the CO₂RR. This higher surface pH is a consequence of larger availability of the uncoordinated amine functionalities on the Cu-PLL electrode surface relative to the other composite electrodes, as shown through X-ray photoelectron spectroscopy.

Original language	English (US)
Pages (from-to)	2993-3002
Number of pages	10
Journal	ACS Applied Energy Materials
Volume	8
Issue number	5
Early online date	Feb 17 2025
DOIs	https://doi.org/10.1021/acsaem.4c03092
State	Published - Mar 10 2025

Keywords

Cu-polymer coordination
composite electrode
electrochemical CO reduction
electrodeposition
polymer
surface pH

ASJC Scopus subject areas

Chemical Engineering (miscellaneous)
Energy Engineering and Power Technology
Electrochemistry
Materials Chemistry
Electrical and Electronic Engineering

Online availability

10.1021/acsaem.4c03092

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Cite this

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title = "Effect of Polymer Variation in Cu-Polymer Composite Electrodes on Electrochemical CO2 Reduction",

abstract = "Cu-polyamine composite electrodes for the CO2RR were prepared using three different amine-functionalized polymers: poly-l-lysine (PLL), poly-l-histidine (PLH), and poly-l-arginine (PLA). Of the composite electrodes, the Cu-PLL electrode demonstrated the highest selectivity for multicarbon (C2+) products, reaching an FEC2+ of 74.3% at −0.98 V vs a reversible hydrogen electrode in a flow cell. In situ surface-enhanced Raman spectroscopy studies obtained from the composite electrodes show that a higher surface pH is achieved on the Cu-PLL electrode during the CO2RR. This higher surface pH is a consequence of larger availability of the uncoordinated amine functionalities on the Cu-PLL electrode surface relative to the other composite electrodes, as shown through X-ray photoelectron spectroscopy.",

keywords = "Cu-polymer coordination, composite electrode, electrochemical CO reduction, electrodeposition, polymer, surface pH",

author = "Wang, {Heryn K.} and Sit, {Chun Yat} and Haasch, {Richard T.} and Kenis, {Paul J.A.} and Gewirth, {Andrew A.}",

note = "H.K.W. acknowledges a Beck State March and Theodore L. Brown Graduate Fellowship from the UIUC Chemistry department. C.Y.B.S. and P.J.A.K would like to acknowledge funding from the Moonshot Research and Development Program (JPNP18016) commissioned by the New Energy and Industrial Technology Development Organization (NEDO).",

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doi = "10.1021/acsaem.4c03092",

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AU - Wang, Heryn K.

AU - Sit, Chun Yat

AU - Haasch, Richard T.

AU - Kenis, Paul J.A.

AU - Gewirth, Andrew A.

N1 - H.K.W. acknowledges a Beck State March and Theodore L. Brown Graduate Fellowship from the UIUC Chemistry department. C.Y.B.S. and P.J.A.K would like to acknowledge funding from the Moonshot Research and Development Program (JPNP18016) commissioned by the New Energy and Industrial Technology Development Organization (NEDO).

PY - 2025/3/10

Y1 - 2025/3/10

N2 - Cu-polyamine composite electrodes for the CO2RR were prepared using three different amine-functionalized polymers: poly-l-lysine (PLL), poly-l-histidine (PLH), and poly-l-arginine (PLA). Of the composite electrodes, the Cu-PLL electrode demonstrated the highest selectivity for multicarbon (C2+) products, reaching an FEC2+ of 74.3% at −0.98 V vs a reversible hydrogen electrode in a flow cell. In situ surface-enhanced Raman spectroscopy studies obtained from the composite electrodes show that a higher surface pH is achieved on the Cu-PLL electrode during the CO2RR. This higher surface pH is a consequence of larger availability of the uncoordinated amine functionalities on the Cu-PLL electrode surface relative to the other composite electrodes, as shown through X-ray photoelectron spectroscopy.

AB - Cu-polyamine composite electrodes for the CO2RR were prepared using three different amine-functionalized polymers: poly-l-lysine (PLL), poly-l-histidine (PLH), and poly-l-arginine (PLA). Of the composite electrodes, the Cu-PLL electrode demonstrated the highest selectivity for multicarbon (C2+) products, reaching an FEC2+ of 74.3% at −0.98 V vs a reversible hydrogen electrode in a flow cell. In situ surface-enhanced Raman spectroscopy studies obtained from the composite electrodes show that a higher surface pH is achieved on the Cu-PLL electrode during the CO2RR. This higher surface pH is a consequence of larger availability of the uncoordinated amine functionalities on the Cu-PLL electrode surface relative to the other composite electrodes, as shown through X-ray photoelectron spectroscopy.

KW - Cu-polymer coordination

KW - composite electrode

KW - electrochemical CO reduction

KW - electrodeposition

KW - polymer

KW - surface pH

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