TY - JOUR
T1 - Synergistic Interaction between the Ni-Center and Glycine-Derived N-Doped Porous Carbon Material Boosts Electrochemical CO2 Reduction
AU - Zhu, Jian
AU - Mulder, Thijs
AU - Rokicińska, Anna
AU - Lindenbeck, Lucie M.
AU - Van den Hoek, Järi
AU - Havenith, Remco W.A.
AU - V. Cunha, Ana
AU - Kuśtrowski, Piotr
AU - Slabon, Adam
AU - Das, Shoubhik
AU - Cool, Pegie
N1 - Publisher Copyright:
© 2024 American Chemical Society.
PY - 2024/7/19
Y1 - 2024/7/19
N2 - 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.
AB - 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.
KW - electrochemical CO2 reduction
KW - hierarchical porous structure
KW - biomass-derived carbon
KW - nickel nanoparticle
KW - nitrogen doping
UR - http://www.scopus.com/inward/record.url?scp=85198056459&partnerID=8YFLogxK
U2 - 10.1021/acscatal.4c00881
DO - 10.1021/acscatal.4c00881
M3 - Article
AN - SCOPUS:85198056459
SN - 2155-5435
VL - 14
SP - 10987
EP - 10997
JO - ACS Catalysis
JF - ACS Catalysis
IS - 14
ER -