Potentialabhängige Morphologie von Kupferkatalysatoren während der Elektroreduktion von CO<sub>2</sub>, ermittelt durch In‐situ‐Rasterkraftmikroskopie

Simon, Géza; Kley, Christopher S.; Cuenya, Beatriz Roldán

doi:10.1002/ange.202010449

Cited by 8 publications

(2 citation statements)

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“…The restructuring of copper‐based catalysts during electrochemical reactions has previously been observed [20,21,37] . Some studies support that upon exposure to reductive potentials, cathodic dissolution is triggered by Cu‐oxide reduction.…”

Section: Resultsmentioning

confidence: 79%

“…However, understanding the reaction dependency on these factors is hindered by the proneness of Cu re‐oxidation and the gradually increasing pH (due to the generation of hydroxyl ions) during the electrochemical reaction [19] . Furthermore, the stability of Cu catalysts in NO 3 − RR is poorly addressed compared with other relevant electrochemical reactions such as carbon dioxide reduction [20,21] …”

Section: Introductionmentioning

confidence: 99%

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Morphology Changes of Cu₂O Catalysts During Nitrate Electroreduction to Ammonia**

et al. 2023

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This manuscript reports the electrosynthesis of ammonia from nitrate catalysed Cu derived from Cu2O materials. Cu2O (111) and (100) preferential grain orientations were prepared through electrodeposition. Cu derived from Cu2O (111) is more active and selective for ammonia formation than Cu2O (100) derived Cu. The highest faradaic efficiency (FE) was achieved for both catalysts at −0.3 V vs RHE, with Cu derived from Cu2O (111) reaching up to 80 %. Additional measurements with quasi‐in situ X‐ray photoelectron spectroscopy and in situ Raman spectroscopy revealed that Cu0 is the active phase during the reaction. The stability of the catalysts was examined by ex situ methods such as SEM, XRD and ICP elemental analysis. The catalysts underwent severe morphological changes as a function of the applied potential and the reaction time, most likely due to the dissolution and redeposition of Cu. After 3 hours of reaction, the entire surface of the catalysts was reconstructed into nanoneedles. The FE after 3 hours remained higher for the Cu derived from Cu2O (111), suggesting that the activity is dependent on the initial structure and the different rates of dissolution and re‐deposition.

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Section: Resultsmentioning

confidence: 79%

Section: Introductionmentioning

confidence: 99%

Morphology Changes of Cu₂O Catalysts During Nitrate Electroreduction to Ammonia**

et al. 2023

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Identifying Structure–Selectivity Correlations in the Electrochemical Reduction of CO₂: A Comparison of Well‐Ordered Atomically Clean and Chemically Etched Copper Single‐Crystal Surfaces

et al. 2021

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The identification of the active sites for the electrochemical reduction of CO2 (CO2RR) to specific chemical products is elusive, owing in part to insufficient data gathered on clean and atomically well‐ordered electrode surfaces. Here, ultrahigh vacuum based preparation methods and surface science characterization techniques are used with gas chromatography to demonstrate that subtle changes in the preparation of well‐oriented Cu(100) and Cu(111) single‐crystal surfaces drastically affect their CO2RR selectivity. Copper single crystals with clean, flat, and atomically ordered surfaces are predicted to yield hydrocarbons; however, these were found experimentally to favor the production of H2. Only when roughness and defects are introduced, for example by electrochemical etching or a plasma treatment, are significant amounts of hydrocarbons generated. These results show that structural and morphological effects are the key factors determining the catalytic selectivity of CO2RR.

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Insight into Structural Evolution, Active Sites, and Stability of Heterogeneous Electrocatalysts

2022

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Studying structure–activity correlations of electrocatalysts is essential for improving the conversion of electrical to chemical energy. Recently, increasing evidence obtained by operando characterization techniques reveal that the structural evolution of catalysts caused by the interplay with electric fields, electrolytes and reactants/intermediates brings about the formation of real active sites. Hence, it is time to summarize structural evolution related research advances and envisage future developments. In this Minireview, we first introduce the fundamental concepts associated with structural evolution (e.g., catalysts, active sites/centers and stability/lifetime) and their relevance. Then, the multiple triggers of structural evolution and advanced operando characterizations are discussed. Significantly, a brief overview of structural evolution and its reversibility in heterogeneous electrocatalysis is provided, especially for the representative electrocatalytic oxygen evolution reaction (OER) and CO2 reduction reaction (CO2RR) processes. Lastly, key challenges and opportunities in this exciting field are highlighted.

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Potentialabhängige Morphologie von Kupferkatalysatoren während der Elektroreduktion von CO₂, ermittelt durch In‐situ‐Rasterkraftmikroskopie

Abstract: Supporting information for this article is given via a link at the end of the document.

Cited by 8 publications

References 103 publications

Morphology Changes of Cu₂O Catalysts During Nitrate Electroreduction to Ammonia**

Morphology Changes of Cu₂O Catalysts During Nitrate Electroreduction to Ammonia**

Identifying Structure–Selectivity Correlations in the Electrochemical Reduction of CO₂: A Comparison of Well‐Ordered Atomically Clean and Chemically Etched Copper Single‐Crystal Surfaces

Insight into Structural Evolution, Active Sites, and Stability of Heterogeneous Electrocatalysts

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Potentialabhängige Morphologie von Kupferkatalysatoren während der Elektroreduktion von CO2, ermittelt durch In‐situ‐Rasterkraftmikroskopie

Abstract: Supporting information for this article is given via a link at the end of the document.

Cited by 8 publications

References 103 publications

Morphology Changes of Cu2O Catalysts During Nitrate Electroreduction to Ammonia**

Morphology Changes of Cu2O Catalysts During Nitrate Electroreduction to Ammonia**

Identifying Structure–Selectivity Correlations in the Electrochemical Reduction of CO2: A Comparison of Well‐Ordered Atomically Clean and Chemically Etched Copper Single‐Crystal Surfaces

Insight into Structural Evolution, Active Sites, and Stability of Heterogeneous Electrocatalysts

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Potentialabhängige Morphologie von Kupferkatalysatoren während der Elektroreduktion von CO₂, ermittelt durch In‐situ‐Rasterkraftmikroskopie

Morphology Changes of Cu₂O Catalysts During Nitrate Electroreduction to Ammonia**

Morphology Changes of Cu₂O Catalysts During Nitrate Electroreduction to Ammonia**

Identifying Structure–Selectivity Correlations in the Electrochemical Reduction of CO₂: A Comparison of Well‐Ordered Atomically Clean and Chemically Etched Copper Single‐Crystal Surfaces