<p>Hydrogen species participate in the whole process of electrochemical CO<sub>2</sub> reduction, which is traditionally treated as a negative factor from the competitive hydrogen evolution reaction. Here, we illustrate for the first time that the rapid transfer of hydrogen species can significantly promote the deep reduction of CO<sub>2</sub> to ethylene products on copper-based catalysts. We construct a hydrogen transfer channel on Cu<sub>2</sub>O nanowires by introducing a conductive copper meso-tetra(4-carboxyphenyl)porphine (Cu-TCPP) layer, where the Cu nodes can adsorb H<sub>2</sub>O and the coordinated carboxyl group can adsorb H<sub>ad</sub> simultaneously. The hydrogen species from the bulk solution are transferred to the CO<sub>2</sub> reduction step by forming H<sub>3</sub>O<sup>+</sup> with target H<sub>2</sub>O and exchanging with the adsorbed H<sub>ad</sub>. Density functional theory (DFT) calculations reveal that the channel eventually facilitates the continuous exothermic hydrogenation reaction of the C<sub>2</sub> intermediate towards ethylene production, which accelerates the ethylene generation with the highest faradic efficiency of 78.6% in neutral conditions in H-cells.</p>

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Hydrogen transfer channel for promoting electroreduction of CO2 to ethylene

  • Bin Lei,
  • Haiqiang Luo,
  • Bo Li,
  • Xiao Liu,
  • Anbang He,
  • Jiapeng Rong,
  • Jian-Gong Ma,
  • Peng Cheng

摘要

Hydrogen species participate in the whole process of electrochemical CO2 reduction, which is traditionally treated as a negative factor from the competitive hydrogen evolution reaction. Here, we illustrate for the first time that the rapid transfer of hydrogen species can significantly promote the deep reduction of CO2 to ethylene products on copper-based catalysts. We construct a hydrogen transfer channel on Cu2O nanowires by introducing a conductive copper meso-tetra(4-carboxyphenyl)porphine (Cu-TCPP) layer, where the Cu nodes can adsorb H2O and the coordinated carboxyl group can adsorb Had simultaneously. The hydrogen species from the bulk solution are transferred to the CO2 reduction step by forming H3O+ with target H2O and exchanging with the adsorbed Had. Density functional theory (DFT) calculations reveal that the channel eventually facilitates the continuous exothermic hydrogenation reaction of the C2 intermediate towards ethylene production, which accelerates the ethylene generation with the highest faradic efficiency of 78.6% in neutral conditions in H-cells.