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Smith, Sean C.
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article
Electroreduction of CO2 to CO on a Mesoporous Carbon Catalyst with Progressively Removed Nitrogen Moieties
Abstract
In this study, we prepared nitrogen-removed mesoporous carbon (NRMC) catalysts by applying various heat treatments to nitrogen-doped mesoporous carbon (NMC), which were applied as novel electrocatalysts for CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR). With the nitrogen moieties being progressively removed, the NRMC catalysts exhibited enhanced CO generation from CO<sub>2</sub>RR, whereas the competing hydrogen evolution reaction (HER) has been suppressed. Through suitable annealing treatment, the defect-rich NRMC catalyst is able to convert CO<sub>2</sub> to CO with a Faradaic efficiency (FE<sub>CO</sub>) of ∼80% and a partial current density for CO ( <i>j</i><sub>CO</sub>) of -2.9 mA cm<sup>-2</sup> at an applied overpotential of 490 mV. Density functional theory (DFT) calculations further revealed the active sites within NRMC catalysts were the defects generated by N removal, which lowered the energy barriers for CO<sub>2</sub>RR and will not be passivated by hydrogen. These findings provide design guidelines to develop efficient carbon-based catalysts that can display metal-like, and even better, performances for potential scalable CO<sub>2</sub>RR to fuels and chemicals.