Synchronous optimization of H2O and H adsorption on NiO1-xTex nanodots for alkaline photocatalytic H2 evolution

[Display omitted] •NiO1-xTex nanodots were constructed by a complexation-photodeposition method.•The H2-production rate of TiO2 can be obviously enhanced by NiO1-xTex cocatalyst.•The electron-deficient Niδ+ and Teδ+ active sites can synchronously enhance the adsorption of H2O and H.•An optimized alkaline H2-production mechanism of NiO1-xTex cocatalyst was proposed. Suitable H2O and H adsorption on the surface of transition metal chalcogenide cocatalyst is highly required to achieve their excellent alkaline H2-evolution rate. However, the weak adsorption of H2O and H atoms on NiTe surface greatly hinders its alkaline H2-evolution efficiency. Herein, an electron-deficient modulation strategy is proposed to synchronously improve the adsorption of H2O and H atoms on NiTe surface, which can greatly improve the alkaline photocatalytic H2 evolution of TiO2. In this case, highly electronegative oxygen atoms are introduced into the NiTe cocatalysts to induce the formation of electron-deficient Niδ+ and Teδ+ sites in the ultra-small-sized NiO1-xTex nanodots (0.5–2 nm), which can be uniformly loaded onto the TiO2 surface to prepare the NiO1-xTex/TiO2 photocatalysts by a facile complexation-photodeposition strategy. The resulting NiO1-xTex/TiO2 (0.6:0.4) photocatalyst exhibits the optimal activity (2143.36 μmol g-1 h−1), surpassing the activity levels of TiO2 and NiTe/TiO2 samples by 42.3 and 1.8 times, respectively. The experimental and theoretical investigations have revealed that the presence of highly electronegative O atoms in the NiO1-xTex cocatalyst can redistribute the charges of Ni and Te atoms for the formation of electron-deficient Niδ+ and Teδ+ active sites, thereby synchronously enhancing the adsorption of H2O on Niδ+ sites and H on Teδ+ sites and promoting alkaline photocatalytic H2 evolution. The current research about the synchronous optimization of the H2O and H adsorption offers a significant approach to design high-performance H2-evolution materials.