Nitrogen-doped carbon nanotube-encapsulated nickel nanoparticles assembled on graphene for efficient CO₂ electroreduction

Exploring 3D hybrid nanocarbons encapsulated with metal nanoparticles (NPs) are recently considered as emerging catalysts for boosting CO₂ electroreduction reaction (CRR) under practical and economic limits. Herein, we report a one-step pyrolysis strategy for fabricating N-doped carbon nanotube (CNT)-encapsulated Ni NPs assembled on the surface of graphene (N/NiNPs@CNT/G) to efficiently convert CO₂ into CO. In such 3D hybrid, the particle size of Ni NPs that coated by five graphitic carbon layers is less than 100 nm, and the amount of N dopants introduced into graphene with countable CNTs is determined to 7.27 at%. Thanks to unique CNT-encapsulated Ni NPs structure and N dopants, the achieved N/NiNPs@CNT/G hybrid displays an exceptional CRR activity with a high Faradaic efficiency of 97.7% and large CO partial current density of 7.9 mA/cm² at −0.7 V, which outperforms those reported metallic NPs loaded carbon based CRR electrocatalysts. Further, a low Tafel slope of 134 mV/dec, a turnover frequency of 387.3 CO/h at −0.9 V, and tiny performance losses during long-term CRR operation are observed on N/NiNPs@CNT/G. Experimental observations illustrate that the Ni NPs encapsulated by carbon layers along with N dopants are of great importance in the conversion of CO₂ into CO with high current density.