Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell

Currently, the electrochemical reduction of carbon dioxide faces significant challenges, including poor selectivity for C<sub>2</sub> products and low conversion efficiency. An effective strategy for optimizing the reduction reaction pathway and enhancing catalytic performance involves m...

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Main Authors: Hanlin Wang, Tian Wang, Gaigai Dong, Linbo Zhang, Fan Pan, Yunqing Zhu
Format: Article
Language:English
Published: MDPI AG 2025-04-01
Series:Inorganics
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Online Access:https://www.mdpi.com/2304-6740/13/5/130
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author Hanlin Wang
Tian Wang
Gaigai Dong
Linbo Zhang
Fan Pan
Yunqing Zhu
author_facet Hanlin Wang
Tian Wang
Gaigai Dong
Linbo Zhang
Fan Pan
Yunqing Zhu
author_sort Hanlin Wang
collection DOAJ
description Currently, the electrochemical reduction of carbon dioxide faces significant challenges, including poor selectivity for C<sub>2</sub> products and low conversion efficiency. An effective strategy for optimizing the reduction reaction pathway and enhancing catalytic performance involves manipulating highly unsaturated atomic sites on the catalyst’s surface, thereby increasing the number of active sites. In this study, we employed sodium dodecylbenzenesulfonate (SDBS) as a surfactant in the electrodeposition method to synthesize copper cubes encapsulated with an amorphous shell (100 nm–250 nm) containing numerous defect sites on its surface. The electrocatalytic CO<sub>2</sub> reduction reactions in an H-type reactor showed that, compared to ED-Cu synthesized without additives, AS (amorphous shell)-Cu-5 exhibited a Faradaic efficiency value for ethylene that was 1.7 times greater than that of ED-Cu while significantly decreasing the Faradaic efficiency of hydrogen production. In situ attenuated total reflectance surface-enhanced infrared spectroscopy (ATR-SEIRAS) revealed that introducing an amorphous shell and abundant defects altered both the intermediate species and reaction pathways on the AS-Cu-5 catalyst’s surface, favoring C<sub>2</sub>H<sub>4</sub> formation. The density functional theory (DFT) calculations further confirmed that amorphous copper lowers the energy barrier required for C-C coupling, resulting in a marked enhancement in FE-C<sub>2</sub>H<sub>4</sub>. Therefore, additive-assisted electrodeposition presents a simple and rapid synthesis method for improving ethylene selectivity in copper catalysts.
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spelling doaj-art-d8004c86475d43f3a231380a6bdda3c02025-08-20T03:47:59ZengMDPI AGInorganics2304-67402025-04-0113513010.3390/inorganics13050130Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous ShellHanlin Wang0Tian Wang1Gaigai Dong2Linbo Zhang3Fan Pan4Yunqing Zhu5School of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi’an 710021, ChinaSchool of Environmental Engineering, Henan University of Technology, Zhengzhou 450001, ChinaSchool of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi’an 710021, ChinaSchool of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi’an 710021, ChinaSchool of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi’an 710021, ChinaSchool of Environmental Science and Engineering, Shaanxi University of Science and Technology, Xi’an 710021, ChinaCurrently, the electrochemical reduction of carbon dioxide faces significant challenges, including poor selectivity for C<sub>2</sub> products and low conversion efficiency. An effective strategy for optimizing the reduction reaction pathway and enhancing catalytic performance involves manipulating highly unsaturated atomic sites on the catalyst’s surface, thereby increasing the number of active sites. In this study, we employed sodium dodecylbenzenesulfonate (SDBS) as a surfactant in the electrodeposition method to synthesize copper cubes encapsulated with an amorphous shell (100 nm–250 nm) containing numerous defect sites on its surface. The electrocatalytic CO<sub>2</sub> reduction reactions in an H-type reactor showed that, compared to ED-Cu synthesized without additives, AS (amorphous shell)-Cu-5 exhibited a Faradaic efficiency value for ethylene that was 1.7 times greater than that of ED-Cu while significantly decreasing the Faradaic efficiency of hydrogen production. In situ attenuated total reflectance surface-enhanced infrared spectroscopy (ATR-SEIRAS) revealed that introducing an amorphous shell and abundant defects altered both the intermediate species and reaction pathways on the AS-Cu-5 catalyst’s surface, favoring C<sub>2</sub>H<sub>4</sub> formation. The density functional theory (DFT) calculations further confirmed that amorphous copper lowers the energy barrier required for C-C coupling, resulting in a marked enhancement in FE-C<sub>2</sub>H<sub>4</sub>. Therefore, additive-assisted electrodeposition presents a simple and rapid synthesis method for improving ethylene selectivity in copper catalysts.https://www.mdpi.com/2304-6740/13/5/130CO<sub>2</sub> electroreductionCu cubeamorphous CuC–C coupling*COCHO intermediate
spellingShingle Hanlin Wang
Tian Wang
Gaigai Dong
Linbo Zhang
Fan Pan
Yunqing Zhu
Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell
Inorganics
CO<sub>2</sub> electroreduction
Cu cube
amorphous Cu
C–C coupling
*COCHO intermediate
title Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell
title_full Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell
title_fullStr Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell
title_full_unstemmed Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell
title_short Boosting C-C Coupling for Electrochemical CO<sub>2</sub> Reduction over Novel Cu-Cubic Catalysts with an Amorphous Shell
title_sort boosting c c coupling for electrochemical co sub 2 sub reduction over novel cu cubic catalysts with an amorphous shell
topic CO<sub>2</sub> electroreduction
Cu cube
amorphous Cu
C–C coupling
*COCHO intermediate
url https://www.mdpi.com/2304-6740/13/5/130
work_keys_str_mv AT hanlinwang boostingcccouplingforelectrochemicalcosub2subreductionovernovelcucubiccatalystswithanamorphousshell
AT tianwang boostingcccouplingforelectrochemicalcosub2subreductionovernovelcucubiccatalystswithanamorphousshell
AT gaigaidong boostingcccouplingforelectrochemicalcosub2subreductionovernovelcucubiccatalystswithanamorphousshell
AT linbozhang boostingcccouplingforelectrochemicalcosub2subreductionovernovelcucubiccatalystswithanamorphousshell
AT fanpan boostingcccouplingforelectrochemicalcosub2subreductionovernovelcucubiccatalystswithanamorphousshell
AT yunqingzhu boostingcccouplingforelectrochemicalcosub2subreductionovernovelcucubiccatalystswithanamorphousshell