April 22 - 26, 2024
Seattle, Washington
May 7 - 9, 2024 (Virtual)

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2024 MRS Spring Meeting
EN09.05.11

Atomic Layer Deposition of Cu Electrocatalysts on Gas Diffusion Electrodes for CO2 Reduction

When and Where

Apr 24, 2024
11:45am - 12:00pm
Room 337, Level 3, Summit

Presenter(s)

Co-Author(s)

Julia Lenef1,Si Young Lee1,Kalyn Fuelling1,Kevin Rivera Cruz1,Aditya Prajapati2,Daniel Delgado Cornejo1,Tae Cho1,Kai Sun1,Eugenio Alvarado1,Timothy Arthur3,Charles Roberts3,Christopher Hahn2,Charles McCrory1,Neil Dasgupta1

University of Michigan1,Lawrence Livermore National Laboratory2,Toyota Research Institute of North America3

Abstract

Julia Lenef1,Si Young Lee1,Kalyn Fuelling1,Kevin Rivera Cruz1,Aditya Prajapati2,Daniel Delgado Cornejo1,Tae Cho1,Kai Sun1,Eugenio Alvarado1,Timothy Arthur3,Charles Roberts3,Christopher Hahn2,Charles McCrory1,Neil Dasgupta1

University of Michigan1,Lawrence Livermore National Laboratory2,Toyota Research Institute of North America3
Electrochemical recycling of carbon dioxide into value-added products is a promising strategy to mitigate climate change as the CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) can be driven using renewable electricity (i.e. wind, solar). So far, copper metal is the only known single element catalyst to form multi-carbon products, such as ethylene and ethanol, from CO<sub>2</sub>RR. Numerous synthesis strategies have been employed to deposit copper-based catalysts including sputtering, evaporation electrodeposition, and solution processing; however, they do not enable atomically precise control of film thickness and particle size and have limited conformality on 3-D substrates such as carbon gas diffusion electrodes. To address this knowledge gap, we fabricate Cu catalysts using plasma-enhanced atomic layer deposition (PE-ALD) with varied PE-ALD cycle numbers on 3D carbon electrodes to achieve precise control of catalyst loading. A polycrystalline Cu metal layer was confirmed by grazing incidence X-ray diffraction. The catalyst surface morphology was probed by scanning electron microscopy and atomic force microscopy, highlighting the island-growth mode of the metal catalyst.<br/><br/>We demonstrate that Cu surfaces prepared by PE-ALD can reduce CO<sub>2</sub>, forming value-added products such as carbon monoxide, methane, and ethylene. Parasitic hydrogen evolution was minimized to Faradaic efficiencies of ~10%, as quantified using <i>in situ</i> gas chromatography measurements. We further demonstrate a selectivity over 40% Faradaic efficiency for ethylene production, which is among the highest values reported to date in an H-cell geometry. Compared to evaporated Cu catalysts, we show significant methane suppression for the PE-ALD Cu. Finally, we demonstrated stability for up to 15 h for CO<sub>2</sub> reduction products with minimum loss in the ethylene production rate. In summary, we demonstrate CO<sub>2</sub>RR using PE-ALD of Cu catalysts with high selectivity and stability, which provides a pathway to conformal deposition on 3D substrates with precise control of particle size and catalyst loading.

Keywords

atomic layer deposition

Symposium Organizers

Christopher Barile, University of Nevada, Reno
Nathalie Herlin-Boime, CEA Saclay
Michel Trudeau, Concordia University
Edmund Chun Ming Tse, University Hong Kong

Session Chairs

Michel Trudeau
Edmund Chun Ming Tse

In this Session