Laser-Microstructured Copper Reveals Selectivity Patterns in the Electrocatalytic Reduction of CO2
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Date
2020-07-09
Publication Type
Journal Article
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yes
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Abstract
The strategy of engineering the local chemical environment to direct selectivity in the electroreduction of CO2 toward value-added products is only qualitatively understood. The unfeasibility of local concentration measurements and the limited applicability of simulations to practical systems hinder more precise guidelines. Herein, we quantify the impact of the (electro)chemical environment on the selectivity pattern using microstructured Cu electrodes prepared by ultrashort pulse laser ablation. We created regularly distributed micro-probes and assessed their product distributions at distinct overpotentials. The regular geometry enabled the accurate simulation of the local pH and CO2 concentration. Selectivity maps useful for mechanistic and applied studies emerged. They reveal clear patterns for C1-C3 products suggesting novel insights such as the presence of two reaction mechanisms for propanol. The effect on the selectivity pattern of operation parameters such as enhanced mass transport and electrolyte composition was also predicted by the maps.
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published
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Book title
Journal / series
Volume
6 (7)
Pages / Article No.
1707 - 1722
Publisher
Elsevier
Event
Edition / version
Methods
Software
Geographic location
Date collected
Date created
Subject
electrocatalysis; CO2 reduction; oxide-derived Cu; laser ablation; microfabrication; local electrochemical environment; selectivity patterns; reaction mechanism
Organisational unit
03871 - Pérez-Ramírez, Javier / Pérez-Ramírez, Javier
03641 - Wegener, Konrad (emeritus) / Wegener, Konrad (emeritus)
Notes
Funding
ETH-47 19-1 - Microstructured electrocatalysts as a design platform for decentralized ammonia synthesis and carbon dioxide fixation in artificial leaves (ETHZ)
732840 - An Artificial Leaf: a photo-electro-catalytic cell from earth-abundant materials for sustainable solar production of CO2-based chemicals and fuels (EC)
169654 - Functional Surface Structuring for Innovative Tools - FuSSI tools (SNF)
732840 - An Artificial Leaf: a photo-electro-catalytic cell from earth-abundant materials for sustainable solar production of CO2-based chemicals and fuels (EC)
169654 - Functional Surface Structuring for Innovative Tools - FuSSI tools (SNF)