Atomically Interfacial Engineering on Molybdenum Nitride Quantum Dots Decorated N-doped Graphene for High-Rate and...

The development of low-cost, high-efficiency, and stable electrocatalysts for hydrogen evolution reaction (HER) under alkaline conditions is a key challenge in water electrolysis. Here, an interfacial engineering strategy that is capable of simultaneously regulating nanoscale structure, electronic structure, and interfacial structure of Mo₂ N quantum dots decorated on conductive N-doped graphene via codoping single-atom Al and O (denoted as AlO@Mo₂ N-NrGO) is reported. The conversion of Anderson polyoxometalates anion cluster ([AlMo₆ O₂₄ H₆ ]^3- , denoted as AlMo6) to Mo₂ N quantum dots not only result in the generation of more exposed active sites but also in situ codoping atomically dispersed Al and O, that can fine-tune the electronic structure of Mo₂ N. It is also identified that the surface reconstruction of AlOH hydrates in AlO@Mo₂ N quantum dots plays an essential role in enhancing hydrophilicity and lowering the energy barriers for water dissociation and hydrogen desorption, resulting in a remarkable alkaline HER performance, even better than the commercial 20% Pt/C. Moreover, the strong interfacial interaction (MoN bonds) between AlO@Mo₂ N and N-doped graphene can significantly improve electron transfer efficiency and interfacial stability. As a result, outstanding stability over 300 h at a current density higher than 100 mA cm^-2 is achieved, demonstrating great potential for the practical application of this catalyst.