Abstract
The ability to synthesize value-added chemicals directly from CO2 will be an important technological advancement for future generations. Using solar energy to drive thermodynamically uphill electrochemical reactions allows for near carbon-neutral processes that can convert CO2 into energy-rich carbon-based fuels. Here, we report on the use of inexpensive CuSn alloys to convert CO2 into CO in an acetonitrile/imidazolium-based electrolyte. Synergistic interactions between the CuSn catalyst and the imidazolium cation enables the electrocatalytic conversion of CO2 into CO at −1.65 V versus the standard calomel electrode (SCE). This catalyst system is characterized by overpotentials for CO2 reduction that are similar to more expensive Au- and Ag-based catalysts, and also shows that the efficacy of the CO2 reduction reaction can be tuned by varying the CuSn ratio.
Highlights
The development of cost-effective systems for the conversion of CO2 into value-added products and high-energy species such as CO and saturated hydrocarbons is of global importance [1,2]
It has been shown that the 2e− /2H+ CO2 reduction reaction (CO2 RR) to generate CO is promoted by metallic cathodes in the presence of imidazolium-based ([Im]+ ) non-aqueous electrolytes [9,10,11,12,13]
As mentioned above, Sn has been shown to facilitate the CO2 reduction reaction (CO2 RR) to generate CO from CO2 dissolved in [Im]+ /MeCN-based electrolytes (j ~ 7.5 mA/cm at −1.95 V vs. standard calomel electrode (SCE)), we considered the ability of Sn-containing alloys to promote the CO2 RR under similar conditions
Summary
The development of cost-effective systems for the conversion of CO2 into value-added products and high-energy species such as CO and saturated hydrocarbons is of global importance [1,2]. It has been shown that the 2e− /2H+ CO2 reduction reaction (CO2 RR) to generate CO is promoted by metallic cathodes in the presence of imidazolium-based ([Im]+ ) non-aqueous electrolytes [9,10,11,12,13]. CO2 electroreduction in [Im]+ -based electrolytes has been shown to occur selectively and efficiently using inexpensive non-noble cathodes such as bismuth [16,17] These metals inhibit the kinetics for the H2 evolution reaction (HER) by increasing the activation energy of the surface hydride formation [18,19]. As mentioned above, Sn has been shown to facilitate the CO2 reduction reaction (CO2 RR) to generate CO from CO2 dissolved in [Im]+ /MeCN-based electrolytes (j ~ 7.5 mA/cm at −1.95 V vs SCE), we considered the ability of Sn-containing alloys to promote the CO2 RR under similar conditions. We compare the activity and selectivity of a pure phase CuSn alloy with one having excess Sn, and document the CO2RR performance of these systems in MeCN containing [BMIM]+ electrolytes
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