Global warming, worldwide energy crisis and the issues related to increasing levels of carbon dioxide (CO2) have prompted the research of new catalysts to transform CO2 back to fuels and value-added chemicals [1]. Copper (Cu)-based nanocatalysts have attracted increasing interest in CO2 reduction over the last decades, due to their unique capability to promote an electrochemical reduction of CO2 into multicarbon C2+ products. Nevertheless, an efficient Cu-catalyst is required to face the typical high overpotentials required for the process and the low selectivity, which results in obtaining a mixture of several products (C1-C3) [2]. Combining molecular with heterogeneous chemistry has revealed to be an efficient approach to improve the efficiency of the CO2RR processes [3]. In fact, the formation of hybrid materials combining heterogeneous Cu-based nanoreactors with organic or metal-organic frameworks allowed to tune stability of key reaction intermediates, enhancing selectivity towards some specific product [4]. In this work, we developed hybrid molecular-heterogeneous Cu-based nanomaterials for CO2RR, with the aim of tunning the selectivity of the nanostructured Cu catalysts by combining them with a purely organic molecularly defined polymer. The design of these systems is based on a novel strategy, whereby cuprous oxide (Cu2O) nanoparticles with a well-defined cubic geometry are used as both, templates and catalyst, for an in-situ polymerization reaction based on azide-alkyne ‘’click’’ reaction between the molecular building blocks. The catalytic performances of the hybrid nanomaterials were tested in a H-type electrochemical cell setup with an online gas-chromatographic quantification analysis (NMR was used for the liquid quantification analysis) and found to be efficient electrocatalysts for CO2RR obtaining a mixture of C1-C2 gaseous products (primarily CO, C2H4, CH4 in addition to H2) and C1-C3 liquids products (primarily C2H6O and CHOO-) in neutral pH electrolyte.
Copper-based hybrid nanomaterials for the electrocatalytic reduction of CO2
Federico Franco;
2023-01-01
Abstract
Global warming, worldwide energy crisis and the issues related to increasing levels of carbon dioxide (CO2) have prompted the research of new catalysts to transform CO2 back to fuels and value-added chemicals [1]. Copper (Cu)-based nanocatalysts have attracted increasing interest in CO2 reduction over the last decades, due to their unique capability to promote an electrochemical reduction of CO2 into multicarbon C2+ products. Nevertheless, an efficient Cu-catalyst is required to face the typical high overpotentials required for the process and the low selectivity, which results in obtaining a mixture of several products (C1-C3) [2]. Combining molecular with heterogeneous chemistry has revealed to be an efficient approach to improve the efficiency of the CO2RR processes [3]. In fact, the formation of hybrid materials combining heterogeneous Cu-based nanoreactors with organic or metal-organic frameworks allowed to tune stability of key reaction intermediates, enhancing selectivity towards some specific product [4]. In this work, we developed hybrid molecular-heterogeneous Cu-based nanomaterials for CO2RR, with the aim of tunning the selectivity of the nanostructured Cu catalysts by combining them with a purely organic molecularly defined polymer. The design of these systems is based on a novel strategy, whereby cuprous oxide (Cu2O) nanoparticles with a well-defined cubic geometry are used as both, templates and catalyst, for an in-situ polymerization reaction based on azide-alkyne ‘’click’’ reaction between the molecular building blocks. The catalytic performances of the hybrid nanomaterials were tested in a H-type electrochemical cell setup with an online gas-chromatographic quantification analysis (NMR was used for the liquid quantification analysis) and found to be efficient electrocatalysts for CO2RR obtaining a mixture of C1-C2 gaseous products (primarily CO, C2H4, CH4 in addition to H2) and C1-C3 liquids products (primarily C2H6O and CHOO-) in neutral pH electrolyte.Pubblicazioni consigliate
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