Dataset Information

Effect of the Cu^2+/1+ Redox Potential of Non-Macrocyclic Cu Complexes on Electrochemical CO₂ Reduction.

ABSTRACT: Cu^2+/1+ complexes facilitate the reduction of CO₂ to valuable chemicals. The catalytic conversion likely involves the binding of CO₂ and/or reduction intermediates to Cu^2+/1+, which in turn could be influenced by the electron density on the Cu^2+/1+ ion. Herein we investigated whether modulating the redox potential of Cu^2+/1+ complexes by changing their ligand structures influenced their CO₂ reduction performance significantly. We synthesised new heteroleptic Cu^2/1+ complexes, and for the first time, studied a (Cu-bis(8-quinolinolato) complex, covering a Cu^2+/1+ redox potential range of 1.3 V. We have found that the redox potential influenced the Faradaic efficiency of CO₂ reduction to CO. However, no correlation between the redox potential and the Faradaic efficiency for methane was found. The lack of correlation could be attributed to the presence of a Cu-complex-derived catalyst deposited on the electrodes leading to a heterogeneous catalytic mechanism, which is controlled by the structure of the in situ deposited catalyst and not the redox potential of the pre-cursor Cu^2+/1+ complexes.

SUBMITTER: Kim K

PROVIDER: S-EPMC10343594 | biostudies-literature | 2023 Jul

REPOSITORIES: biostudies-literature

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Effect of the Cu2+/1+ Redox Potential of Non-Macrocyclic Cu Complexes on Electrochemical CO2 Reduction.

Kim Kyuman K Wagner Pawel P Wagner Klaudia K Mozer Attila J AJ

Molecules (Basel, Switzerland) 20230703 13

Cu2+/1+ complexes facilitate the reduction of CO2 to valuable chemicals. The catalytic conversion likely involves the binding of CO2 and/or reduction intermediates to Cu2+/1+, which in turn could be influenced by the electron density on the Cu2+/1+ ion. Herein we investigated whether modulating the redox potential of Cu2+/1+ complexes by changing their ligand structures influenced their CO2 reduction performance signifi ...[more]

PMID: 37446840

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Project description:The electrochemical CO2 reduction reaction (CO2RR) holds enormous potential as a carbon-neutral route to the sustainable production of fuels and platform chemicals. The durability for long-term operation is currently inadequate for commercialization, however, and the underlying deactivation process remains elusive. A fundamental understanding of the degradation mechanism of electrocatalysts, which can dictate the overall device performance, is needed. In this work, we report the structural dynamics and degradation pathway of Cu oxide nanoparticles (CuOx NPs) during the CO2RR by using in situ small-angle X-ray scattering (SAXS) and X-ray absorption spectroscopy (XAS). The in situ SAXS reveals a reduction in the size of NPs when subjected to a potential at which no reaction products are detected. At potentials where the CO2RR starts to occur, CuOx NPs are agglomerated through a particle migration and coalescence process in the early stage of the reaction, followed by Ostwald ripening (OR) as the dominant degradation mechanism for the remainder of the reaction. As the applied potential becomes more negative, the OR process becomes more dominant, and for the most negative applied potential, OR dominates for the entire reaction time. The morphological changes are linked to a gradual decrease in the formation rate for multicarbon products (C2H4 and ethanol). Other reaction parameters, including reaction intermediates and local high pH, induce changes in the agglomeration process and final morphology of the CuOx NPs electrode, supported by post-mortem ex situ microscopic analysis. The in situ XAS analysis suggests that the CuOx NPs reduced into the metallic state before the structural transformation was observed. The introduction of high surface area carbon supports with ionomer coating mitigates the degree of structural transformation and detachment of the CuOx NPs electrode. These findings show the dynamic nature of Cu nanocatalysts during the CO2RR and can serve as a rational guideline toward a stable catalyst system under electrochemical conditions.

Dataset Information

Effect of the Cu^2+/1+ Redox Potential of Non-Macrocyclic Cu Complexes on Electrochemical CO₂ Reduction.

Publications

Effect of the Cu<sup>2+/1+</sup> Redox Potential of Non-Macrocyclic Cu Complexes on Electrochemical CO<sub>2</sub> Reduction.

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