Journal
SMALL
Volume 19, Issue 30, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202300049
Keywords
coordination environments; porous structures; single Ni atoms; CO2 reduction; electrocatalysis
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Tuning the coordination environment and geometric structures of single atom catalysts is an effective approach for maximizing catalytic efficiency. A template-based synthesis strategy was proposed in this study to synthesize high-density NiNx sites on the surface of nitrogen-doped carbon nanofibers. The results showed that the dual engineering strategy increased the number of active sites and utilization efficiency of each single atom, resulting in superior catalytic activity and selectivity for CO2 reduction reactions.
Tuning the coordination environment and geometric structures of single atom catalysts is an effective approach for regulating the reaction mechanism and maximize the catalytic efficiency of single-atom centers. Here, a template-based synthesis strategy is proposed for the synthesis of high-density NiNx sites anchored on the surface of hierarchically porous nitrogen-doped carbon nanofibers (Ni-HPNCFs) with different coordination environments. First-principles calculations and advanced characterization techniques demonstrate that the single Ni atom is strongly coordinated with both pyrrolic and pyridinic N dopants, and that the predominant sites are stabilized by NiN3 sites. This dual engineering strategy increases the number of active sites and utilization efficiency of each single atom as well as boosts the intrinsic activity of each active site on a single-atom scale. Notably, the Ni-HPNCF catalyst achieves a high CO Faradaic efficiency (FECO) of 97% at a potential of -0.7 V, a high CO partial current density (j(CO)) of 49.6 mA cm(-2) (-1.0 V), and a remarkable turnover frequency of 24 900 h(-1) (-1.0 V) for CO2 reduction reactions (CO2RR). Density functional theory calculations show that compared to pyridinic-type NiNx, the pyrrolic-type NiN3 moieties display a superior CO2RR activity over hydrogen evolution reactions, resulting in their superior catalytic activity and selectivity.
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