Understanding the origin of formation and active sites of oxygen evolution reaction (OER) cocatalysts is highly required for solar photoelectrochemical (PEC) devices that generate hydrogen efficiently from water. Herein, we employed a simple pH‐modulated method for in situ growth of FeNi oxyhydroxide ultrathin layers on BiVO4 photoanodes, resulting in one of the highest currently known PEC activities of 5.8 mA cm−2 (1.23 VRHE, AM 1.5 G) accompanied with an excellent stability. More importantly, both comparative experiments and density functional theory (DFT) studies clearly reveal that the selective formation of Bi−O−Fe interfacial bonds mainly contributes the enhanced OER activities, while the construction of V−O−Ni interfacial bonds effectively restrains the dissolution of V5+ ions and promotes the OER stability. Thereby, the synergy between iron and nickel of FeNi oxyhydroxides significantly improved the PEC water oxidation properties of BiVO4 photoanodes.
Ordered mesoporous tricompound NiO−CaO−Al 2 O 3 composite oxides with various Ca content were first designed and facilely synthesized via a one-pot, evaporation-induced, self-assembly (EISA) strategy. The obtained mesoporous materials with advantageous textural properties and superior thermal stabilities were investigated as the catalysts for the carbon dioxide reforming of methane reaction. These mesoporous catalysts entirely showed high catalytic activities as well as long catalytic stabilities toward this reaction. The improved catalytic activities were suggested to be closely associated with the advantageous structural properties, such as large specific surface areas; big pore volumes; and uniform pore sizes, which could provide sufficient "accessible" active centers for the gaseous reactants. In addition, the "confinement effect" of the mesoporous matrixes contributed to stabilizing the Ni active sites during the processes of reduction and reaction, accounting for the long lifetime stabilities of these mesoporous catalysts. The modification of Ca played dual roles in promoting the catalytic activities and suppressing the carbon deposition by enhancing the chemisorption of the CO 2 . Generally, the ordered mesoporous NiO−CaO−Al 2 O 3 composite oxides could be considered as promising catalysts for the carbon dioxide reforming of methane reaction.
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