H2O及其中间体在缺电子Mn(3+δ)+位的自发增强吸附及其促进光催化产H2O2性能OA北大核心CSTPCD

Transitional metal oxyhydroxides have been demonstrated to be the reliable cocatalysts for water oxidation reaction.However,their insufficient adsorption ability for H2O and its intermediate products during water oxidation greatly restricts the improvement of water oxidation rate.In this study,a spontaneously improved adsorption of H2O and its intermediates on the electron-deficient Mn(3+δ)+of MnOOH cocatalyst can greatly promote the rapid water oxidation to realize the efficient photocatalytic H2O2 production in a pure water system.In this case,amorphous MnOOH is selectively deposited on the(110)facet of AuPd-modified single-crystal BiVO4 photocatalyst via the directionally photoinduced oxidation approach to produce AuPd/BiVO4/MnOOH photocatalyst.Photocatalytic experiments exhibit that the as-prepared AuPd/BiVO4/MnOOH(0.5％)photocatalyst obtains the boosted H2O2-evolution rate of 214 µmol·L-1 as well as exhibits an outstanding stability and reproducibility.Density functional theory calculations and X-ray photoelectron spectroscopy(XPS)characterization reveal that the free electrons of MnOOH can effectively transfer to BiVO4 to induce the generation of electron-deficient Mn sites(Mn(3+δ)+),which spontaneously promotes the adsorption of H2O and its intermediates for enhancing 4-electron water oxidation reaction,resulting in an efficient H2O2 production.The present work about the strong interaction between cocatalyst and bulk catalyst provides a fresh idea for the rational design of highly efficient catalytic materials.