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

Department of Applied Chemistry

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

7 Scopus citations

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
Number of pages	9
Journal	Chem Catalysis
Volume	2
Issue number	4
DOIs	https://doi.org/10.1016/j.checat.2022.03.016
State	Published - 21 Apr 2022

Keywords

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

UN SDGs

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

Access to Document

10.1016/j.checat.2022.03.016

Cite this

@article{b413bad0569b4470a15ddd473f3a7675,

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 CO reduction reaction, flow cells, methane, SDG13: Climate action, SDG7: Affordable and clean energy",

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

note = "Publisher Copyright: {\textcopyright} 2022 Elsevier Inc.",

year = "2022",

month = apr,

day = "21",

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

language = "English",

volume = "2",

pages = "908--916",

journal = "Chem Catalysis",

issn = "2667-1107",

publisher = "Cell Press",

number = "4",

}

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 CO reduction reaction

KW - flow cells

KW - methane

KW - SDG13: Climate action

KW - SDG7: Affordable and clean energy

UR - http://www.scopus.com/inward/record.url?scp=85128357280&partnerID=8YFLogxK

U2 - 10.1016/j.checat.2022.03.016

DO - 10.1016/j.checat.2022.03.016

M3 - Article

AN - SCOPUS:85128357280

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

Keywords

UN SDGs

Access to Document

Other files and links

Fingerprint

Cite this