Carbon dioxide (CO2) is a waste product of combustion, it can also be a potential source provided an efficient means to convert it to useful products. A desired catalyst would be active to reduce CO2 selectively to generate desirable products, and stable to obtain high current densities over long period of time. Herein we report a common element, nanostructured catalyst for the direct electrochemical conversion of CO2 to ethanol with high Faradaic efficiency and high selectivity that operates in water and at ambient temperature and pressure.1 We electrochemically deposit Cu nanoparticles on nitrogen-doped carbon nanospike (CNS) electrode, which was prepared via plasma enhanced chemical vapor deposition (PECVD) in the presence of acetylene (C2H2) and ammonia (NH3).2 Nanosized Cu is an efficient metal catalyst for formation of significant amounts of hydrocarbon from CO2 electroreduction.3, 4 Additionally, density functional theory plus dispersion (DFT-D) calculations revealed highly selective adsorption of CO2 by pyridinic nitrogen-doped carbon.5 The catalyst is comprised of Cu nanoparticle on a highly textured, N-doped graphene film. The combination of nitrogen-doped CNS with nanosized Cu is expected to synergistically improve activity and selectivity for CO2 reduction reaction. Detailed electrochemical analysis and complementary DFT calculations indicate a novel mechanism in which multiple active sites, working sequentially, control the coupling of carbon monoxide radicals and mediate the subsequent electrochemical reduction to alcohol.

Copper nanoparticle/carbon nanospike catalyst for high-selectivity electrochemical conversion of carbon dioxide

253rd National Meeting (2017)

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