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

• Published in: ACS catalysis 2024-07, Vol.14 (14), p.10987-10997
• Main Authors: Zhu, Jian, Mulder, Thijs, Rokicińska, Anna, Lindenbeck, Lucie M., Van den Hoek, Järi, Havenith, Remco W. A., V. Cunha, Ana, Kuśtrowski, Piotr, Slabon, Adam, Das, Shoubhik, Cool, Pegie
• Format: Article
• Language: English
• ISSN: 2155-5435; 2155-5435
• DOI: 10.1021/acscatal.4c00881

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 (j co) 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.