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• W2955112809 abstract "Copper is one of the most effective catalysts for electrochemically reducing CO and CO2 to useful products. However, the copper surface changes during prolonged electrolysis. To better understand these changes and how they affect the reaction, we performed in situ differential electrochemical mass spectrometry and infrared spectroscopy to monitor the change in volatile products and adsorbates generated over the course of the reaction. During CO reduction at a copper electrode for a series of consecutive cyclic voltammograms (CVs), if the anodic potential limit of the CV does not oxidize the electrode (−0.3 V vs standard hydrogen electrode), in NaHCO3, methane generation initially decreases and multicarbon product (C2 products) generation initially increases. Periodically oxidizing the electrode surface by sweeping the electrode potential to 0.1 V causes surface roughening that decreases the generation of hydrogen over time but keeps the relative amounts of C1 and C2 the same. When the reaction is carried out in CsHCO3 solution, the initial quantity of C2 products is higher. However, the signals corresponding to each kind of product decay after a few minutes of potential cycling. The rapid loss of activity in CsHCO3 suggests accelerated accumulation of products on the electrode surface under this condition. Potential-dependent IR spectra recorded at the electrode surface during a single CV show that, in CsHCO3 solution, the surface coverage of CO is lower than in NaHCO3, whereas the CH coverage is higher.In addition, a band at 1850 cm–1, which suggests the presence of a carbonyl-containing species, is accumulated over consecutive potential cycles. This suggests more rapid generation of adsorbed hydrocarbons in CsHCO3. These results show that multiple mechanisms contribute to the change in product selectivity over time and the dominant mechanism depends upon the specific reaction conditions." @default.
• W2955112809 created "2019-07-12" @default.
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• W2955112809 date "2019-06-26" @default.
• W2955112809 modified "2023-10-18" @default.
• W2955112809 title "Stability of Product Generation during CO Reduction on Copper" @default.
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• W2955112809 doi "https://doi.org/10.1021/acs.jpcc.9b03651" @default.
• W2955112809 hasPublicationYear "2019" @default.
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