Photocatalytic water splitting provides an economically feasible way for converting solar energy into hydrogen. Great efforts have been devoted to developing efficient photocatalysts;however,the surface catalytic reactions,especially for the sluggish oxygen evolution reaction (OER), still remain ac hallenge,w hich limits the overall photocatalytic energy efficiency.Herein, we design aRh n cluster cocatalyst, with Rh 0 -Rh 3+ sites anchoring the Mo-doped BiVO 4 model photocatalytic system. The resultant photocatalyst enables ahigh visiblelight photocatalytic oxygen production activity of 7.11 mmol g À1 h À1 and an apparent quantum efficiency of 29.37 %a t4 20 nm. The turnover frequency (TOF) achieves 416.73 h À1 ,w hich is 378 times higher than that of the photocatalyst only with Rh 3+ species.O perando X-ray absorption characterization shows the OER process on the Rh 0 -Rh 3+ sites. The DFT calculations further illustrate ab ifunctional OER mechanism over the Rh 0 -Rh 3+ sites,i nw hicht he oxygen intermediate attacks the Rh 3+ sites with assistance of ahydrogen atom transfer to the Rh 0 sites,t hus breaking the scaling relationship of various oxygen intermediates.
Free-standing conical BiVO4 crystals featuring a curved surface and sharp tips were synthesized. The sample exhibited an enlarged visible light absorption region and good photocatalytic water oxidation ability.
Bifunctional Rh 0 -Rh 3+ sites … … anchored on Mo-doped BiVO 4 show a high visible-light photocatalytic oxygen production activity, as reported by Peng Fei Liu, Zheng Jiang, Hua Gui Yang, and coworkers in their Research Article on page 22761. Operando XAFS results and DFT calculations illustrate the bifunctional OER mechanism on the Rh 0 -Rh 3+ sites: the oxygen intermediate attacks the Rh 3+ sites, facilitating a hydrogen atom transfer to the adjacent Rh 0 sites, which synergistically optimizes the OER energetics.
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