Loading Single-Ni Atoms on Assembled Hollow N-Rich Carbon Plates for Efficient CO₂ Electroreduction

The rational design of catalysts’ spatial structure is vitally important to boost catalytic performance through exposing the active sites, enhancing the mass transfer, and confining the reactants. Herein, a dual-linker zeolitic tetrazolate framework-engaged strategy is developed to construct assembled hollow plates (AHP) of N-rich carbon (NC), which is loaded with single-Ni atoms to form a highly efficient electrocatalyst (designated as Ni-NC(AHP)). In the carbonization process, the thermally unstable linker (5-aminotetrazole) serves as the self-sacrificial template and the other linker (2-methylimidazole) mainly serves as the carbon and nitrogen source to form hollow NC matrix. The formed Ni-NC(AHP) catalyst possesses enhanced mesoporosity and more available surface area, thus promoting mass transport and affording abundant accessible single-Ni sites. These features contribute to remarkable performance for electrochemical CO₂ reduction with exceptionally high selectivity of nearly 100% towards CO in a wide potential range and dramatically enhanced CO partial current density. © 2021 Wiley-VCH GmbH