Low-dimensional N-heterocyclic carbenes nanomaterials: Promising supports of single atom catalysts

Abstract

The exploration of excellent supports of single-atom catalysts (SACs) has attracted significant attention in catalysis science and technology. Here, we successfully designed a series of low-dimensional N-heterocyclic carbenes nanomaterials (NCMs) as novel supports for SACs with NHCs as coordinating environment of the metal active center. Through first-principles calculations, the obtained NCMs were found to be thermally and dynamically stable, and possess a range of electronic properties from metallic to semiconducting, with one of them exhibiting Dirac cones in the band structures. These NCMs not only maintain the classic characteristics of NHC molecules, but also display new amphoteric properties. Moreover, Fe-adsorbed two-dimensional NCM as an example was found to be an effective SAC for the reduction of N2 molecule with an onset potential of −0.66 V, indicating that NHCs coordination environment can improve the catalytic performance of SACs. This work not only develops a series of novel supports for SACs with NHCs coordinating environment, but also provides a useful strategy of support regulation to enhance the catalytic performance of SACs.