Abstract
A fundamental question in the electrochemical CO2 reduction reaction is how to rationally control its catalytic selectivity, for example, how to convert CO2 to hydrocarbons or oxygenates. In this presentation, we shall share our latest work on this theme to make multi-carbon oxygenates such as ethanol, propanol, etc. We shall illustrate this with several examples. One of them is by creating highly defective Cu sites. The other is by adding a CO-producing metal like Ag to Cu. We found that the CuAg boundaries in the composites facilitate the coupling of carbon-containing species to give ethanol. Specifically, oxide-derived Cu nanowires mixed with 20 nm Ag particles reduce CO2 to ethanol with a current density of -4.1 mA/cm2 at -1.1 V vs. RHE and ethanol/ethylene Faradaic efficiency ratio of 1.1. These figures of merit are respectively 5 and 3 times higher than those for pure oxide-derived Cu nanowires. Extensive experimentations and DFT calculations shows selective ethanol evolution via Langmuir-Hinshelwood *CO + *CHx (x = 1, 2) coupling at CuAg boundaries. The formation of energy-intensive CO dimers can be circumvented.
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