Ni5Ga3 catalysts for CO2 reduction to methanol: Exploring the role of Ga surface oxidation/reduction on catalytic activity

Gallo, Alessandro; Snider, Jonathan L.; Sokaras, Dimosthenis; Nordlund, Dennis; Kröll, Thomas; Ogasawara, Hirohito; Kovařík, Libor; Duyar, Melis S.; Jaramillo, Thomas F.

doi:10.1016/j.apcatb.2019.118369

Cited by 78 publications

(65 citation statements)

References 72 publications

(106 reference statements)

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“…For example, metals such as tin (Sn), zinc (Zn), and indium (In) were reported to catalyze the reduction of CO 2 to oxygen‐containing C 1 products, including formate (HCOO – ) and CO. [ 28–35 ] However, techno‐economic analyses suggest that reduction to yield liquid alcohols (e.g., methanol, ethanol, and propanol) and ethylene gas (C 2 H 4 ) is likely required to make the process of CO 2 reduction economically viable. [ 36,37 ]…”

Section: Introductionmentioning

confidence: 99%

“…[ 49,59–70 ] CuAg bimetallic catalysts are particularly important and reported to have increased conductivity, stability, and local concentration of surface carbon monoxide species (CO*). [ 15,16,36,43,65–68,70 ] Research on CuAg catalysts often relies on large nanoparticles (NPs, >30 nm), likely due to the challenges for making bimetallic NPs between two immiscible metals, highlighting the synthetic need and importance for controlling the atomic ratio and nanostructures between Cu and Ag towards generating active sites. [ 65–67,70 ] Strain effects of Ag atoms on the surface of CuAg nanocrystals may also promote multi‐carbon products.…”

Section: Introductionmentioning

confidence: 99%

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Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C₂₊ Chemicals from Carbon Dioxide at Low Cell Potentials

Kuhn

Zhao

Nwabara

et al. 2021

Adv Funct Materials

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Copper catalysts are widely studied for the electroreduction of carbon dioxide (CO2) to value‐added hydrocarbon products. Controlling the surface composition of copper nanomaterials may provide the electronic and structural properties necessary for carbon‐carbon coupling, thus increasing the Faradaic efficiency (FE) towards ethylene and other multi‐carbon (C2+) products. Synthesis and catalytic study of silver‐coated copper nanoparticles (Cu@Ag NPs) for the reduction of CO2 are presented. Bimetallic CuAg NPs are typically difficult to produce due to the bulk immiscibility between these two metals. Slow injection of the silver precursor, concentrations of organic capping agents, and gas environment proved critical to control the size and metal distribution of the Cu@Ag NPs. The optimized Cu@Ag electrocatalyst exhibited a very low onset cell potential of −2.25 V for ethylene formation, reaching a FE towards C2+ products (FEC2+) of 43% at −2.50 V, which is 1.0 V lower than a reference Cu catalyst to reach a similar FEC2+. The high ethylene formation at low potentials is attributed to enhanced CC coupling on the Ag enriched shell of the Cu@Ag electrocatalysts. This study offers a new catalyst design towards increasing the efficiency for the electroreduction of CO2 to value‐added chemicals.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C₂₊ Chemicals from Carbon Dioxide at Low Cell Potentials

Kuhn

Zhao

Nwabara

et al. 2021

Adv Funct Materials

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“…On the basis of theoretical considerations, the reactivity has been attributed to the formation of Ga-rich metallic sites. 2 On the other hand, Ga is prone to oxidation, 4 thus resulting in a Ga oxide shell, surrounding a metallic core of nanoparticles (NPs), 5 which can only be reduced in hydrogen at high temperatures.…”

Section: Introductionmentioning

confidence: 99%

Structural Evolution of Ga–Cu Model Catalysts for CO₂ Hydrogenation Reactions

2021

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We studied the initial stages of Ga interaction with the Cu(001) surface and environment-induced surface transformations in an attempt to elucidate the surface chemistry of the Cu–Ga catalysts recently proposed for CO2 hydrogenation to methanol. The results show that Ga readily intermixes with Cu upon deposition in vacuum. However, even traces of oxygen in the gas ambient cause Ga oxidation and the formation of two-dimensional (“monolayer”) Ga oxide islands uniformly covering the Cu surface. The surface morphology and the oxidized state of Ga remain in H2 as well as in a CO2 + H2 reaction mixture at elevated pressures and temperatures (0.2 mbar, 700 K). The results indicate that the Ga-doped Cu surface under reaction conditions exposes a variety of structures including GaO x /Cu interfacial sites, which must be taken into account for elucidating the reaction mechanism.

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“…Metallic gallium is incorporated into the nickel lattice to form an intermetallic phase. A recent work reveals that the Ga‐oxide shell surrounding the metallic core is formed via Ga migrating from the subsurface region to the surface of the nanoparticles when exposed to air [53c] . The surface oxidized Ni 5 Ga 3 is more active than fully reduced Ni 5 Ga 3 for methanol synthesis.…”

Section: Bimetallic Catalysts For Co2 Hydrogenation To Methanolmentioning

confidence: 99%

Hydrogenation of Carbon Dioxide to Methanol over Non−Cu‐based Heterogeneous Catalysts

et al. 2020

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Ni5Ga3 catalysts for CO2 reduction to methanol: Exploring the role of Ga surface oxidation/reduction on catalytic activity

Cited by 78 publications

References 72 publications

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C₂₊ Chemicals from Carbon Dioxide at Low Cell Potentials

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C₂₊ Chemicals from Carbon Dioxide at Low Cell Potentials

Structural Evolution of Ga–Cu Model Catalysts for CO₂ Hydrogenation Reactions

Hydrogenation of Carbon Dioxide to Methanol over Non−Cu‐based Heterogeneous Catalysts

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Ni5Ga3 catalysts for CO2 reduction to methanol: Exploring the role of Ga surface oxidation/reduction on catalytic activity

Cited by 78 publications

References 72 publications

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C2+ Chemicals from Carbon Dioxide at Low Cell Potentials

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C2+ Chemicals from Carbon Dioxide at Low Cell Potentials

Structural Evolution of Ga–Cu Model Catalysts for CO2 Hydrogenation Reactions

Hydrogenation of Carbon Dioxide to Methanol over Non−Cu‐based Heterogeneous Catalysts

Contact Info

Product

Resources

About

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C₂₊ Chemicals from Carbon Dioxide at Low Cell Potentials

Engineering Silver‐Enriched Copper Core‐Shell Electrocatalysts to Enhance the Production of Ethylene and C₂₊ Chemicals from Carbon Dioxide at Low Cell Potentials

Structural Evolution of Ga–Cu Model Catalysts for CO₂ Hydrogenation Reactions