NH4Cl-assisted preparation of single Ni sites anchored carbon nanosheet catalysts for highly efficient carbon dioxide electroreduction

Ping, Dan, Yi, Feng, Zhang, Guiwei, Wu, Shide, Fang, Shaoming, Hu, Kailong, Xu, Bin, Ren, Junna and Guo, Zhanhu (2023) NH4Cl-assisted preparation of single Ni sites anchored carbon nanosheet catalysts for highly efficient carbon dioxide electroreduction. Journal of Materials Science and Technology, 142. pp. 1-9. ISSN 1005-0302

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Abstract

Single-atomic transition metal-nitrogen codoped carbon (M-N-C) are efficient substitute catalysts for noble metals to catalyze electrochemical CO2 reduction reaction. However, the uncontrolled aggregations of metal and serious loss of nitrogen species constituting the M-Nx active sites are frequently observed in the commonly used pyrolysis procedure. Herein, single-atomic nickel (Ni)-based sheet-like electrocatalysts with abundant Ni-N4 active sites were created by using a novel ammonium chloride (NH4Cl)-assited pyrolysis method. Spherical aberration correction electron microscopy and X-ray absorption fine structure analysis clearly revealed that Ni species are atomically dispersed and anchored by N in Ni-N4 structure. The addition of ammonium chloride (NH4Cl) optimized the mesopore size to 7-10 nm, and increased the concentrations of pyridinic N (3.54 wt) and Ni-N4 (3.33 wt) species. The synergistic catalytic effect derived from Ni-N4 active sites and pyridinic N species achieved an outstanding CO2RR performance, presenting a high CO Faradaic efficiency (FECO) up to 98 and a large CO partial current density of 8.5 mA·cm−2 at a low potential of -0.62 V vs. RHE. Particularly, the FECO maintains above 80 within a large potential range from -0.43 to -0.73 V vs. RHE. This work provides a practical and feasible approach to build highly active single-atomic catalysts for CO2 conversion systems.

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