First-Principles Investigation of β-FeOOH for Hydrogen Evolution: Identifying Reactive Sites and Boosting Surface Reactions.

Akaganeite (β-FeOOH) is a widely investigated candidate for photo(electro)catalysis, such as water splitting. Nevertheless, insights into understanding the surface reaction between water and β-FeOOH, in particular, the hydrogen evolution reaction (HER), are still insufficient. Herein, a set of first-principles calculations on pristine β-FeOOH and halogen-substituted β-FeOOH are applied to evaluate the HER performance through the computational hydrogen electrode model. The results show that the HER on β-FeOOH tends to occur at Fe sites on the (010) surface, and palladium and nickel are found to serve as excellent co-catalysts to boost the HER process, due to the remarkably reduced free energy change of hydrogen adsorption upon loading on the surface of β-FeOOH, demonstrating great potential for efficient water splitting.