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Understanding the reaction mechanisms of well-defined metal-N4 sites in electrocatalytic CO2 reduction.

08:00 EDT 12th October 2018 | BioPortfolio

Summary of "Understanding the reaction mechanisms of well-defined metal-N4 sites in electrocatalytic CO2 reduction."

Electrocatalytic CO2 reduction to CO emerges as a potential route of utilizing the excessively emitted CO2. Metal-N-C hybrid structures have shown unique activities, of which the active centers and reaction mechanisms, however, remain unclear due to the ambiguity in true atomic structures for prepared catalysts. Herein, combining density functional theory calculations and experimental studies, we explored the reaction mechanisms on well-defined metal-N4 sites by using metal phthalocyanines as model catalysts. Our theoretical calculations reveal that cobalt phthalocyanine exhibits the optimum activity for CO2 reduction to CO, because of the moderate *CO binding energy on the Co site which accommodates the *COOH formation and the *CO desorption. It is further confirmed by experimental studies, where cobalt phthalocyanine delivers the best performance, with a maximal CO Faradaic efficiency reaching 99%, and maintains the stable performance for over 60 hours.

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Name: Angewandte Chemie (International ed. in English)
ISSN: 1521-3773
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