Abstract

The electrochemical CO2 reduction reaction (CO2RR) to syngas represents a promising solution to mitigate CO2 emissions and manufacture value-added chemicals. Palladium (Pd) has been identified as a potential candidate for syngas production via CO2RR due to its transformation to Pd hydride under CO2RR conditions, however, the pre-hydridized effect on the catalytic properties of Pd-based electrocatalysts has not been investigated. Herein, pre-hydridized Pd nanocubes (PdH0.40) supported on carbon black (PdH0.40 NCs/C) are directly prepared from a chemical reduction method. Compared with Pd nanocubes (Pd NCs/C), PdH0.40 NCs/C presented an enhanced CO2RR performance due to its less cathodic phase transformation revealed by the in situ X-ray absorption spectroscopy. Density functional theory calculations revealed different binding energies of key reaction intermediates on PdH0.40 NCs/C and Pd NCs/C. Study of the size effect further suggests that NCs of smaller sizes show higher activity due to their more abundant active sites (edge and corner sites) for CO2RR. The pre-hydridization and reduced NC size together lead to significantly improved activity and selectivity of CO2RR.

Original languageEnglish
Article number2005305
JournalSmall
Volume16
Issue number49
DOIs
StatePublished - 10 Dec 2020

Keywords

  • carbon dioxide reduction reaction (CO RR)
  • density functional theory (DFT)
  • nanocubes
  • palladium hydride (PdH )
  • syngas

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