Highly selective CO₂ electroreduction to CO by the synergy between Ni-N-C and encapsulated Ni nanoparticles

Efficient catalysts are highly desirable for the selective electrochemical CO₂ reduction reaction (CO₂RR). Ni single-atom catalysts are known as promising CO₂RR catalysts, while Ni NPs are expected to catalyze the competing HER. In this work, we have modified the Ni NPs by encapsulating them into porous Ni-N-C nanosheets (Ni@Ni-N-C), to boost the synergy between Ni NPs and dispersed Ni-N species towards CO₂RR. The CO faradaic efficiency (FE_CO) reached 96.4% at −0.9 V and retained over 90% in a wide potential window. More importantly, FE_CO values of over 94% have been obtained from −50 to −170 mA cm⁻² with a peak FE_CO of 99% in a flow cell. Our work demonstrates that the surface modification of Ni NPs can inhibit the unexpected HER and activate the surface sites, offering a practical design strategy for CO₂RR catalysts.