Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts

Armin Sedighian Rasouli; Xue Wang; Joshua Wicks; Cao-Thang Dinh; Jehad Abed; Feng-Yi Wu; Sung-Fu Hung; Koen Bertens; Jianan Erick Huang; Edward H. Sargent

doi:10.1016/j.checat.2022.03.016

Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts

Armin Sedighian Rasouli, Xue Wang, Joshua Wicks, Cao-Thang Dinh, Jehad Abed, Feng-Yi Wu, Sung-Fu Hung, Koen Bertens, Jianan Erick Huang, Edward H. Sargent^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

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Abstract

The electrochemical CO₂ reduction reaction (CO₂RR) provides a route to store intermittent electricity in the form of fuels like methane. We reasoned that disrupting C-C coupling while maintaining high ∗CO coverage could enhance methane selectivity and suppress the hydrogen evolution reaction (HER). We studied the effect of doping CuAl, a material at the top of the CO₂RR activity and selectivity volcano plot, with elements having low ∗CO binding energies: Au, Zn, and Ga. Encouraged by initial improvements in selectivity to methane, we optimized the Ga content and showed that the presence of uniformly dispersed Ga is crucial in CO₂RR-to-methane performance enhancement. We rule out porosity and roughness and conclude that the presence of Ga in the doped catalysts enables high methane selectivity. The Ga-doped CuAl catalysts achieve a methane Faradaic efficiency (FE) of 53% by suppressing HER to 23% in neutral electrolyte at −1.4 V versus reversible hydrogen electrode.

Original language	English
Pages (from-to)	908-916
Journal	Chem Catalysis
Volume	2
Issue number	4
Online published	12 Apr 2022
DOIs	https://doi.org/10.1016/j.checat.2022.03.016
Publication status	Published - 21 Apr 2022
Externally published	Yes

Research Keywords

Cu-based ternary catalysts
electrochemical CO2 reduction reaction
flow cells
methane
SDG13: Climate action
SDG7: Affordable and clean energy

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This full text is made available under CC-BY-NC-ND 4.0. https://creativecommons.org/licenses/by-nc-nd/4.0/

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

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title = "Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts",

abstract = "The electrochemical CO2 reduction reaction (CO2RR) provides a route to store intermittent electricity in the form of fuels like methane. We reasoned that disrupting C-C coupling while maintaining high ∗CO coverage could enhance methane selectivity and suppress the hydrogen evolution reaction (HER). We studied the effect of doping CuAl, a material at the top of the CO2RR activity and selectivity volcano plot, with elements having low ∗CO binding energies: Au, Zn, and Ga. Encouraged by initial improvements in selectivity to methane, we optimized the Ga content and showed that the presence of uniformly dispersed Ga is crucial in CO2RR-to-methane performance enhancement. We rule out porosity and roughness and conclude that the presence of Ga in the doped catalysts enables high methane selectivity. The Ga-doped CuAl catalysts achieve a methane Faradaic efficiency (FE) of 53% by suppressing HER to 23% in neutral electrolyte at −1.4 V versus reversible hydrogen electrode.",

keywords = "Cu-based ternary catalysts, electrochemical CO2 reduction reaction, flow cells, methane, SDG13: Climate action, SDG7: Affordable and clean energy",

author = "{Sedighian Rasouli}, Armin and Xue Wang and Joshua Wicks and Cao-Thang Dinh and Jehad Abed and Feng-Yi Wu and Sung-Fu Hung and Koen Bertens and Huang, {Jianan Erick} and Sargent, {Edward H.}",

year = "2022",

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doi = "10.1016/j.checat.2022.03.016",

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TY - JOUR

T1 - Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts

AU - Sedighian Rasouli, Armin

AU - Wang, Xue

AU - Wicks, Joshua

AU - Dinh, Cao-Thang

AU - Abed, Jehad

AU - Wu, Feng-Yi

AU - Hung, Sung-Fu

AU - Bertens, Koen

AU - Huang, Jianan Erick

AU - Sargent, Edward H.

PY - 2022/4/21

Y1 - 2022/4/21

N2 - The electrochemical CO2 reduction reaction (CO2RR) provides a route to store intermittent electricity in the form of fuels like methane. We reasoned that disrupting C-C coupling while maintaining high ∗CO coverage could enhance methane selectivity and suppress the hydrogen evolution reaction (HER). We studied the effect of doping CuAl, a material at the top of the CO2RR activity and selectivity volcano plot, with elements having low ∗CO binding energies: Au, Zn, and Ga. Encouraged by initial improvements in selectivity to methane, we optimized the Ga content and showed that the presence of uniformly dispersed Ga is crucial in CO2RR-to-methane performance enhancement. We rule out porosity and roughness and conclude that the presence of Ga in the doped catalysts enables high methane selectivity. The Ga-doped CuAl catalysts achieve a methane Faradaic efficiency (FE) of 53% by suppressing HER to 23% in neutral electrolyte at −1.4 V versus reversible hydrogen electrode.

AB - The electrochemical CO2 reduction reaction (CO2RR) provides a route to store intermittent electricity in the form of fuels like methane. We reasoned that disrupting C-C coupling while maintaining high ∗CO coverage could enhance methane selectivity and suppress the hydrogen evolution reaction (HER). We studied the effect of doping CuAl, a material at the top of the CO2RR activity and selectivity volcano plot, with elements having low ∗CO binding energies: Au, Zn, and Ga. Encouraged by initial improvements in selectivity to methane, we optimized the Ga content and showed that the presence of uniformly dispersed Ga is crucial in CO2RR-to-methane performance enhancement. We rule out porosity and roughness and conclude that the presence of Ga in the doped catalysts enables high methane selectivity. The Ga-doped CuAl catalysts achieve a methane Faradaic efficiency (FE) of 53% by suppressing HER to 23% in neutral electrolyte at −1.4 V versus reversible hydrogen electrode.

KW - Cu-based ternary catalysts

KW - electrochemical CO2 reduction reaction

KW - flow cells

KW - methane

KW - SDG13: Climate action

KW - SDG7: Affordable and clean energy

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U2 - 10.1016/j.checat.2022.03.016

DO - 10.1016/j.checat.2022.03.016

M3 - RGC 21 - Publication in refereed journal

SN - 2667-1107

VL - 2

SP - 908

EP - 916

JO - Chem Catalysis

JF - Chem Catalysis

IS - 4

ER -

Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts

Abstract

Research Keywords

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