Metal-Oxide Interfaces for Selective Electrochemical C-C Coupling Reactions

Chan Woo Lee; Seung Jae Shin; Hyejin Jung; Dang Le Tri Nguyen; Si Young Lee; Woong Hee Lee; Da Hye Won; Min Gyu Kim; Hyung Suk Oh; Taehwan Jang; Hyungjun Kim; Byoung Koun Min; Yun Jeong Hwang

doi:10.1021/acsenergylett.9b01721

Metal-Oxide Interfaces for Selective Electrochemical C-C Coupling Reactions

Chan Woo Lee, Seung Jae Shin, Hyejin Jung, Dang Le Tri Nguyen, Si Young Lee, Woong Hee Lee, Da Hye Won, Min Gyu Kim, Hyung Suk Oh, Taehwan Jang, Hyungjun Kim, Byoung Koun Min, Yun Jeong Hwang

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

81 Citations (Scopus)

Abstract

Metal-oxide interfaces provide a new opportunity to improve catalytic activity based on electronic and chemical interactions at the interface. Constructing a high density of interfaces is essential in maximizing synergistic interactions. Here, we demonstrate that Cu-ceria interfaces made by sintering nanocrystals facilitate C-C coupling reactions in electrochemical reduction of CO₂. The Cu/ceria catalyst enhances the selectivity of ethylene and ethanol production with the suppression of H₂ evolution in comparison with Cu catalysts. The intrinsic activity for ethylene production is enhanced by decreasing the atomic ratio of Cu/Ce, revealing the Cu atoms near ceria are an active site for C-C coupling reactions. The ceria is proposed to weaken the hydrogen binding energy of adjacent Cu sites and stabilize an OCCO intermediate via an additional chemical interaction with an oxygen atom of the OCCO. This work offers new insights into the role of the metal-oxide interface in the electrochemical reduction of CO₂ to high-value chemicals.

Original language	English
Pages (from-to)	2241-2248
Number of pages	8
Journal	ACS Energy Letters
Volume	4
Issue number	9
DOIs	https://doi.org/10.1021/acsenergylett.9b01721
Publication status	Published - 2019 Sept 13

Bibliographical note

Funding Information:
This work was supported by Korea Institute of Science and Technology (KIST) institutional program and the YU-KIST convergence program, and it was also supported by “Next Generation Carbon Upcycling Project” (Project No. 2017M1A2A2046713) through the National Research Foundation (NRF) funded by the Ministry of Science and ICT, Republic of Korea. The authors thank the Pohang Accelerator Laboratory for providing the synchrotron radiation sources at the 10C beamline. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2016R1A5A1012966 and No. 2019R1A2C2005521).

Funding Information:
This work was supported by Korea Institute of Science and Technology (KIST) institutional program and the YU-KIST convergence program, and it was also supported by "Next Generation Carbon Upcycling Project" (Project No. 2017M1A2A2046713) through the National Research Foundation (NRF) funded by the Ministry of Science and ICT, Republic of Korea. The authors thank the Pohang Accelerator Laboratory for providing the synchrotron radiation sources at the 10C beamline. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2016R1A5A1012966 and No. 2019R1A2C2005521).

Publisher Copyright:
Copyright © 2019 American Chemical Society.

ASJC Scopus subject areas

Chemistry (miscellaneous)
Renewable Energy, Sustainability and the Environment
Fuel Technology
Energy Engineering and Power Technology
Materials Chemistry

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acsenergylett.9b01721

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title = "Metal-Oxide Interfaces for Selective Electrochemical C-C Coupling Reactions",

abstract = "Metal-oxide interfaces provide a new opportunity to improve catalytic activity based on electronic and chemical interactions at the interface. Constructing a high density of interfaces is essential in maximizing synergistic interactions. Here, we demonstrate that Cu-ceria interfaces made by sintering nanocrystals facilitate C-C coupling reactions in electrochemical reduction of CO2. The Cu/ceria catalyst enhances the selectivity of ethylene and ethanol production with the suppression of H2 evolution in comparison with Cu catalysts. The intrinsic activity for ethylene production is enhanced by decreasing the atomic ratio of Cu/Ce, revealing the Cu atoms near ceria are an active site for C-C coupling reactions. The ceria is proposed to weaken the hydrogen binding energy of adjacent Cu sites and stabilize an OCCO intermediate via an additional chemical interaction with an oxygen atom of the OCCO. This work offers new insights into the role of the metal-oxide interface in the electrochemical reduction of CO2 to high-value chemicals.",

author = "Lee, {Chan Woo} and Shin, {Seung Jae} and Hyejin Jung and Nguyen, {Dang Le Tri} and Lee, {Si Young} and Lee, {Woong Hee} and Won, {Da Hye} and Kim, {Min Gyu} and Oh, {Hyung Suk} and Taehwan Jang and Hyungjun Kim and Min, {Byoung Koun} and Hwang, {Yun Jeong}",

note = "Funding Information: This work was supported by Korea Institute of Science and Technology (KIST) institutional program and the YU-KIST convergence program, and it was also supported by “Next Generation Carbon Upcycling Project” (Project No. 2017M1A2A2046713) through the National Research Foundation (NRF) funded by the Ministry of Science and ICT, Republic of Korea. The authors thank the Pohang Accelerator Laboratory for providing the synchrotron radiation sources at the 10C beamline. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2016R1A5A1012966 and No. 2019R1A2C2005521). Funding Information: This work was supported by Korea Institute of Science and Technology (KIST) institutional program and the YU-KIST convergence program, and it was also supported by {"}Next Generation Carbon Upcycling Project{"} (Project No. 2017M1A2A2046713) through the National Research Foundation (NRF) funded by the Ministry of Science and ICT, Republic of Korea. The authors thank the Pohang Accelerator Laboratory for providing the synchrotron radiation sources at the 10C beamline. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2016R1A5A1012966 and No. 2019R1A2C2005521). Publisher Copyright: Copyright {\textcopyright} 2019 American Chemical Society.",

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doi = "10.1021/acsenergylett.9b01721",

language = "English",

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journal = "ACS Energy Letters",

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T1 - Metal-Oxide Interfaces for Selective Electrochemical C-C Coupling Reactions

AU - Lee, Chan Woo

AU - Shin, Seung Jae

AU - Jung, Hyejin

AU - Nguyen, Dang Le Tri

AU - Lee, Si Young

AU - Lee, Woong Hee

AU - Won, Da Hye

AU - Kim, Min Gyu

AU - Oh, Hyung Suk

AU - Jang, Taehwan

AU - Kim, Hyungjun

AU - Min, Byoung Koun

AU - Hwang, Yun Jeong

N1 - Funding Information: This work was supported by Korea Institute of Science and Technology (KIST) institutional program and the YU-KIST convergence program, and it was also supported by “Next Generation Carbon Upcycling Project” (Project No. 2017M1A2A2046713) through the National Research Foundation (NRF) funded by the Ministry of Science and ICT, Republic of Korea. The authors thank the Pohang Accelerator Laboratory for providing the synchrotron radiation sources at the 10C beamline. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2016R1A5A1012966 and No. 2019R1A2C2005521). Funding Information: This work was supported by Korea Institute of Science and Technology (KIST) institutional program and the YU-KIST convergence program, and it was also supported by "Next Generation Carbon Upcycling Project" (Project No. 2017M1A2A2046713) through the National Research Foundation (NRF) funded by the Ministry of Science and ICT, Republic of Korea. The authors thank the Pohang Accelerator Laboratory for providing the synchrotron radiation sources at the 10C beamline. This work was supported by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2016R1A5A1012966 and No. 2019R1A2C2005521). Publisher Copyright: Copyright © 2019 American Chemical Society.

PY - 2019/9/13

Y1 - 2019/9/13

N2 - Metal-oxide interfaces provide a new opportunity to improve catalytic activity based on electronic and chemical interactions at the interface. Constructing a high density of interfaces is essential in maximizing synergistic interactions. Here, we demonstrate that Cu-ceria interfaces made by sintering nanocrystals facilitate C-C coupling reactions in electrochemical reduction of CO2. The Cu/ceria catalyst enhances the selectivity of ethylene and ethanol production with the suppression of H2 evolution in comparison with Cu catalysts. The intrinsic activity for ethylene production is enhanced by decreasing the atomic ratio of Cu/Ce, revealing the Cu atoms near ceria are an active site for C-C coupling reactions. The ceria is proposed to weaken the hydrogen binding energy of adjacent Cu sites and stabilize an OCCO intermediate via an additional chemical interaction with an oxygen atom of the OCCO. This work offers new insights into the role of the metal-oxide interface in the electrochemical reduction of CO2 to high-value chemicals.

AB - Metal-oxide interfaces provide a new opportunity to improve catalytic activity based on electronic and chemical interactions at the interface. Constructing a high density of interfaces is essential in maximizing synergistic interactions. Here, we demonstrate that Cu-ceria interfaces made by sintering nanocrystals facilitate C-C coupling reactions in electrochemical reduction of CO2. The Cu/ceria catalyst enhances the selectivity of ethylene and ethanol production with the suppression of H2 evolution in comparison with Cu catalysts. The intrinsic activity for ethylene production is enhanced by decreasing the atomic ratio of Cu/Ce, revealing the Cu atoms near ceria are an active site for C-C coupling reactions. The ceria is proposed to weaken the hydrogen binding energy of adjacent Cu sites and stabilize an OCCO intermediate via an additional chemical interaction with an oxygen atom of the OCCO. This work offers new insights into the role of the metal-oxide interface in the electrochemical reduction of CO2 to high-value chemicals.

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U2 - 10.1021/acsenergylett.9b01721

DO - 10.1021/acsenergylett.9b01721

M3 - Article

AN - SCOPUS:85072328410

SN - 2380-8195

VL - 4

SP - 2241

EP - 2248

JO - ACS Energy Letters

JF - ACS Energy Letters

IS - 9

ER -

Metal-Oxide Interfaces for Selective Electrochemical C-C Coupling Reactions

Abstract

Bibliographical note

ASJC Scopus subject areas

UN SDGs

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