Synergistic Interaction between the Ni-Center and Glycine-Derived N-Doped Porous Carbon Material Boosts Electrochemical CO2 Reduction

Jian Zhu, Thijs Mulder, Anna Rokicińska, Lucie M. Lindenbeck, Järi Van den Hoek, Remco W.A. Havenith, Ana V. Cunha, Piotr Kuśtrowski, Adam Slabon, Shoubhik Das*, Pegie Cool*

*Corresponding author for this work

Research output: Contribution to journalArticleAcademicpeer-review

4 Citations (Scopus)

Abstract

Electrochemical conversion of CO2 into CO is highly attractive since CO is highly valuable for its wide use in organic synthesis as well as a fuel-type molecule. However, the selective formation of CO from CO2 is highly sensitive to the variation of particle size, coordination number, and defects in the electrocatalyst. Considering this, we report a boosted electrochemical CO2 reduction performance on a Ni, N-codoped hierarchical porous carbon material (Ni@MicroPNC) by exposing substantial active sites during the carbonization process by using ZnCl2 as the porous template agent due to its relatively low boiling point. A particular advantage of our electrocatalyst is that the support (N-doped hierarchical porous carbon material) of the Ni-catalyst is synthesized by using glycine as a carbon precursor. To our observation, the as-prepared Ni@MicroPNC catalyst displayed a high CO faradaic efficiency (FE) of 92.8% with a high partial current density (jCO) of 22.4 mA cm-2 and outstanding current density stability at −0.81 V (vs RHE) for 10 h. The suggested high CO selectivity and catalytic stability of Ni@MicroPNC are attributed to the synergistic effect of high specific surface area, optimized hierarchical structure, Ni, N codoping into the porous carbon material, and relatively weaker CO binding strength. Furthermore, DFT calculations indicate that the doped N atom interacted with the Ni center to lower the energy barrier of *CO desorption. This finding provides a facile strategy for the synthesis of low-cost and highly active nanoparticle-based electrocatalysts for a selective reduction of CO2 into CO.

Original languageEnglish
Pages (from-to)10987-10997
Number of pages11
JournalACS Catalysis
Volume14
Issue number14
Early online date8-Jul-2024
DOIs
Publication statusPublished - 19-Jul-2024

Keywords

  • electrochemical CO2 reduction
  • hierarchical porous structure
  • biomass-derived carbon
  • nickel nanoparticle
  • nitrogen doping

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