Cu@Cr 2 O 3 Noble‐Metal‐Free Hydrogen‐Evolving Cocatalyst on Al‐Doped SrTiO 3 for Photocatalytic Overall Water Splitting

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ABSTRACT The development of noble‐metal‐free cocatalysts is crucial for low‐cost photocatalytic overall water splitting (POWS) systems. However, dynamic structural evolution of non‐noble‐metal materials under operando conditions results in a restricted activity of cocatalysts in POWS. Herein, we construct a core–shell structured Cu@Cr 2 O 3 cocatalyst on Al‐doped SrTiO 3 (SrTiO 3 :Al) via a photodeposition method (denoted as Cu‐PD/STO) for efficient H 2 evolution in POWS. The Cu‐PD/STO achieves the H 2 evolution rate of 788.7 µmol/h, surpassing all the recently reported noble‐metal‐free H 2 evolution cocatalysts on SrTiO 3 for POWS. Quasi in situ/ operando characterizations elucidate the stable operation of Cu 0 active sites in POWS, guaranteed by the photoinduced reduction of Cu sites and core–shell structure. Further characterizations and theoretical calculations reveal that Cu 0 active sites provide accelerated electron extraction from SrTiO 3 :Al, optimized water dissociation, and hydrogen adsorption. Moreover, Cu 0 active sites can promote the formation of Cr 2 O 3 shells, which encapsulate the Cu 0 active sites, protecting them against surface oxidation and suppressing the reverse reaction in POWS.

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