Abstract: Strain engineering of two-dimensional (2D) material interfaces represents a powerful strategy for enhancing the electrocatalytic activity of water splitting. However, maintaining catalytic stability under various harsh conditions by introducing interface strain remains a great challenge. The catalyst developed and evaluated herein comprised Ir clusters dispersed on 2D NiO nanosheets (NSs) derived from metal organic frameworks (Ir@NiO/C_BDC), which displays a high activity and stability under all pH conditions, and even a change of only 1% in the applied voltage is observed after continuous electrocatalytic operation for over 1800 h under alkaline conditions. Through combined experimental and computational studies, we found that the introduced interfacial strain contributes to the outstanding structural stability of the Ir@NiO/C_BDC catalyst, arising from its increased Ir and Ni vacancy formation energies, and hence suppressing its leaching. Moreover, strain also enhances the kinetically sluggish electrocatalytic water splitting reaction by optimizing its electronic structure and coordination environment. This work highlights the effects of strain on catalyst stability and provides new insights for designing widely applicable electrocatalysts.

Key words: Strain engineering, Stability, Electrocatalysts, Two-dimensional material, Water splitting