Synthesis of N-Doped Highly Graphitic Carbon Urchin-Like Hollow Structures Loaded with Single-Ni Atoms towards Efficient CO₂ Electroreduction

The rational design of single-atom catalysts featuring excellent conductivity, highly accessible discrete active sites and favorable mass transfer is crucial for electrocatalysis but remains challenging. In this study, a reliable Ni-catalyzed and Ni-templated strategy is developed to synthesize a single-atom catalyst by transforming metallic Ni into single-Ni atoms anchored on hollow porous urchin-like (HPU) N-doped carbon (NC) (designated as Ni-NC(HPU)), which possesses high crystallinity and sufficient Ni-N₄ moiety (2.4 wt %). The unique hollow thorns on the surface, good conductivity and large external surface area facilitate electron/mass transfer and exposure of single-Ni sites. As a result, the Ni-NC(HPU) catalyst exhibits remarkable activity and high stability for CO₂ electroreduction. Moreover, this synthetic strategy can also be facilely extended to prepare distinct hollow porous architectures with similar components, such as the wire- and sphere-like ones. © 2022 Wiley-VCH GmbH.