Changeable Active Sites by Pr Doping CuSA‐TiO 2 Photocatalyst for Excellent Hydrogen Production

Abstract Photocatalytic water splitting for clean hydrogen production has been a very attractive research field for decades. However, the insightful understanding of the actual active sites and their impact on catalytic performance is still ambiguous. Herein, a Pr‐doped TiO 2 ‐supported Cu single atom (SA) photocatalyst is successfully synthesized (noted as Cu/Pr‐TiO 2 ). It is found that Pr dopants passivate the formation of oxygen vacancies, promoting the density of photogenerated electrons on the CuSAs, and optimizing the electronic structure and H * adsorption behavior on the CuSA active sites. The photocatalytic hydrogen evolution rate of the obtained Cu/Pr‐TiO 2 catalyst reaches 32.88 mmol g −1 h −1 , 2.3 times higher than the Cu/TiO 2 . Innovatively, the excellent catalytic activity and performance is attributed to the active sites change from O atoms to CuSAs after Pr doping is found. This work provides new insight for understanding the accurate roles of single atoms in photocatalytic water splitting.