The electrochemical reduction of carbon dioxide (CO2) holds tremendous promise as a sustainable pathway to mitigate greenhouse gas emissions while producing valuable chemical feedstocks and fuels. However, the development of efficient catalysts for this process remains a significant challenge. Traditional bulk catalysts often suffer from limited selectivity, poor activity, and high overpotentials. Single atom catalysts (SACs) have gained enormous interest in recent years due to their unique electronic and geometric properties, offering new possibilities for enhancing catalytic efficiency in CO2 reduction reactions. In this context, recent data show how the addition of axial ligands on the metal site located in defect sites of carbon-based conductive networks represents an effective strategy to promote various electrochemical reactions. In this work we explore through DFT calculations how the presence of axial ligands (e.g. atoms or small molecules) introduced through simple organic reactions can influence the metal geometry and electronic characteristics, modifying the overall energy of the reaction and the selectivity of the CO2RR to CO or other products.
Theoretical insights on innovative solutions for CO2RR with Single Atom Catalysts
Giuseppe SANTORIELLO;Ida RITACCO;Giuliano GIAMBASTIANI;Lucia CAPORASO
2024
Abstract
The electrochemical reduction of carbon dioxide (CO2) holds tremendous promise as a sustainable pathway to mitigate greenhouse gas emissions while producing valuable chemical feedstocks and fuels. However, the development of efficient catalysts for this process remains a significant challenge. Traditional bulk catalysts often suffer from limited selectivity, poor activity, and high overpotentials. Single atom catalysts (SACs) have gained enormous interest in recent years due to their unique electronic and geometric properties, offering new possibilities for enhancing catalytic efficiency in CO2 reduction reactions. In this context, recent data show how the addition of axial ligands on the metal site located in defect sites of carbon-based conductive networks represents an effective strategy to promote various electrochemical reactions. In this work we explore through DFT calculations how the presence of axial ligands (e.g. atoms or small molecules) introduced through simple organic reactions can influence the metal geometry and electronic characteristics, modifying the overall energy of the reaction and the selectivity of the CO2RR to CO or other products.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
