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Growth Dynamics and Processes Governing the Stability of Electrodeposited Size-Controlled Cubic Cu Catalysts

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posted on 26.11.2020, 13:36 by Philipp Grosse, Aram Yoon, Clara Rettenmaier, See Wee Chee, Beatriz Roldan Cuenya
The renewable energy-powered conversion of industrially generated CO2 into useful chemicals and fuels is considered a promising technology for the sustainable development of our modern society. The electrochemical reduction of CO2 (CO2RR) is one of the possible conversion processes that can be employed to close the artificial carbon cycle, mimicking nature’s photosynthesis. Nevertheless, to enable green catalytic processes, selectivity for the desired products must be achieved. In the case of CO2RR, the selectivity is strongly dependent on the electrocatalyst structure. Here, we explore the phase space of synthesis parameters required for the electrodeposition of Cu cubes with {100} facets on glassy carbon substrates and elucidate their influence on the size, shape, coverage, and uniformity of the cubes. We found that the concentration of Cl ions in solution controls the cube size, shape, and coverage, whereas the ratio of the reduction versus oxidation time and number of cycles in the alternating potential electrodeposition protocol can be used to further tune the cube size. Cyclic voltammetry experiments were complemented with in situ electrochemical scanning electron microscopy to follow the growth dynamics and ex situ transmission electron microscopy and electron diffraction. Our results indicate that the cube growth starts from nuclei formed during the first cycle, followed by a layered deposition and partial dissolution of new material in subsequent cycles.

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