LAUSR

In this work, alkaline hydrogen evolution reaction (HER) processes of three typical nickel-based electrocatalysts, i.e., Ni, α-Ni(OH) 2 , and β-Ni(OH) 2 , were investigated to probe critical factors that determine the activity and durability. The HER activity trend is observed as Ni >> α-Ni(OH) 2 > β-Ni(OH) 2 , likely attributed to a synergy between metallic Ni and Ni(OH) 2 components on the Ni surface and fast water dissociation kinetics on the α-Ni(OH) 2 surface. With the HER proceeding, the metallic Ni surface, however, gradually becomes α-Ni(OH) 2 , and α-Ni(OH) 2 surface ultimately transforms into β-phase, leading to a dramatic activity decrease of Ni electrodes. Therefore, we coated Ni electrodes with α-Ni(OH) 2 nanosheets to slow down the nickel hydroxylation and optimise the surface ratio of Ni(OH) 2 to metallic Ni. This simple coating procedure enhances both activity and durability of Ni electrocatalysts.