Electrodeposited CuAgHg Multimetallic Thin Films for Improved CO2Conversion: The Dramatic Impact of Hg Incorporation on Product Selectivity

Joo Yeon Kim; C. Hyun Ryu; Jeong Heon Lee; Amol U. Pawar; Woo Dong Jang; Young Soo Kang; Hyun S. Ahn

doi:10.1021/acsaem.0c00784

Electrodeposited CuAgHg Multimetallic Thin Films for Improved CO₂Conversion: The Dramatic Impact of Hg Incorporation on Product Selectivity

Joo Yeon Kim, C. Hyun Ryu, Jeong Heon Lee, Amol U. Pawar, Woo Dong Jang, Young Soo Kang, Hyun S. Ahn

Department of Chemistry

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

12 Citations (Scopus)

Abstract

The CO2 reduction reaction (CO2RR) remains a prominent hurdle in the overall solar to fuel conversion process. A key research direction for CO2RR is tuning of the product selectivity to desired fuels while suppressing the undesired hydrogen-evolving side reaction. In this work, we employed a CuAgHg multimetallic thin-film catalyst for CO2RR. By incorporation of Hg atoms, we attempted to minimize the surface-adsorbed hydrogen atoms during CO2RR, thereby minimizing hydrogen evolution. In situ electrochemical surface interrogation along with vibrational spectroscopy revealed that Hg incorporation led to significantly suppressed surface adsorption of hydrogen atoms, as well as increased surface concentration of the intermediate CO, which is in competitive binding with protons. The two effects combined led to an ethanol-selective CO2RR catalyst; with the optimum composition, the CuAgHg electrode produced 32% ethanol and 41% C2 (ethanol + ethylene) products, comparable to those of the best catalysts reported. Remarkably, this catalysis was possible holding the hydrogen evolving side reaction to mere 10% and achieving 100% overall faradaic efficiency.

Original language	English
Pages (from-to)	6670-6677
Number of pages	8
Journal	ACS Applied Energy Materials
Volume	3
Issue number	7
DOIs	https://doi.org/10.1021/acsaem.0c00784
Publication status	Published - 2020 Jul 27

Bibliographical note

Funding Information:
This work was financially supported by the Basic Science Research Program through the National Research Foundation (NRF) of Korea (NRF-2020R1C1C1007409 and NRF-2019M3E6A1064707).

Publisher Copyright:
Copyright © 2020 American Chemical Society.

All Science Journal Classification (ASJC) codes

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

Access to Document

10.1021/acsaem.0c00784

Cite this

@article{0dfa05dfbb08420381f230aa668ce7c4,

title = "Electrodeposited CuAgHg Multimetallic Thin Films for Improved CO2Conversion: The Dramatic Impact of Hg Incorporation on Product Selectivity",

abstract = "The CO2 reduction reaction (CO2RR) remains a prominent hurdle in the overall solar to fuel conversion process. A key research direction for CO2RR is tuning of the product selectivity to desired fuels while suppressing the undesired hydrogen-evolving side reaction. In this work, we employed a CuAgHg multimetallic thin-film catalyst for CO2RR. By incorporation of Hg atoms, we attempted to minimize the surface-adsorbed hydrogen atoms during CO2RR, thereby minimizing hydrogen evolution. In situ electrochemical surface interrogation along with vibrational spectroscopy revealed that Hg incorporation led to significantly suppressed surface adsorption of hydrogen atoms, as well as increased surface concentration of the intermediate CO, which is in competitive binding with protons. The two effects combined led to an ethanol-selective CO2RR catalyst; with the optimum composition, the CuAgHg electrode produced 32% ethanol and 41% C2 (ethanol + ethylene) products, comparable to those of the best catalysts reported. Remarkably, this catalysis was possible holding the hydrogen evolving side reaction to mere 10% and achieving 100% overall faradaic efficiency.",

author = "Kim, {Joo Yeon} and Ryu, {C. Hyun} and Lee, {Jeong Heon} and Pawar, {Amol U.} and Jang, {Woo Dong} and Kang, {Young Soo} and Ahn, {Hyun S.}",

note = "Funding Information: This work was financially supported by the Basic Science Research Program through the National Research Foundation (NRF) of Korea (NRF-2020R1C1C1007409 and NRF-2019M3E6A1064707). Publisher Copyright: Copyright {\textcopyright} 2020 American Chemical Society.",

year = "2020",

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doi = "10.1021/acsaem.0c00784",

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T2 - The Dramatic Impact of Hg Incorporation on Product Selectivity

AU - Kim, Joo Yeon

AU - Ryu, C. Hyun

AU - Lee, Jeong Heon

AU - Pawar, Amol U.

AU - Jang, Woo Dong

AU - Kang, Young Soo

AU - Ahn, Hyun S.

N1 - Funding Information: This work was financially supported by the Basic Science Research Program through the National Research Foundation (NRF) of Korea (NRF-2020R1C1C1007409 and NRF-2019M3E6A1064707). Publisher Copyright: Copyright © 2020 American Chemical Society.

PY - 2020/7/27

Y1 - 2020/7/27

N2 - The CO2 reduction reaction (CO2RR) remains a prominent hurdle in the overall solar to fuel conversion process. A key research direction for CO2RR is tuning of the product selectivity to desired fuels while suppressing the undesired hydrogen-evolving side reaction. In this work, we employed a CuAgHg multimetallic thin-film catalyst for CO2RR. By incorporation of Hg atoms, we attempted to minimize the surface-adsorbed hydrogen atoms during CO2RR, thereby minimizing hydrogen evolution. In situ electrochemical surface interrogation along with vibrational spectroscopy revealed that Hg incorporation led to significantly suppressed surface adsorption of hydrogen atoms, as well as increased surface concentration of the intermediate CO, which is in competitive binding with protons. The two effects combined led to an ethanol-selective CO2RR catalyst; with the optimum composition, the CuAgHg electrode produced 32% ethanol and 41% C2 (ethanol + ethylene) products, comparable to those of the best catalysts reported. Remarkably, this catalysis was possible holding the hydrogen evolving side reaction to mere 10% and achieving 100% overall faradaic efficiency.

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