An electron-hole rich dual-site nickel catalyst for efficient photocatalytic overall water splitting

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Abstract
Photocatalysis offers an attractive strategy to upgrade H2O to renewable fuel H2. However, current photocatalytic hydrogen production technology often relies on additional sacrificial agents and noble metal cocatalysts, and there are limited photocatalysts possessing overall water splitting performance on their own. Here, we successfully construct an efficient catalytic system to realize overall water splitting, where hole-rich nickel phosphides (Ni2P) with polymeric carbon-oxygen semiconductor (PCOS) is the site for oxygen generation and electron-rich Ni2P with nickel sulfide (NiS) serves as the other site for producing H2. The electron-hole rich Ni2P based photocatalyst exhibits fast kinetics and a low thermodynamic energy barrier for overall water splitting with stoichiometric 2:1 hydrogen to oxygen ratio (150.7 μmol h−1H2and 70.2 μmol h−1O2produced per 100 mg photocatalyst) in a neutral solution. Density functional theory calculations show that the co-loading in Ni2P and its hybridization with PCOS or NiS can effectively regulate the electronic structures of the surface active sites, alter the reaction pathway, reduce the reaction energy barrier, boost the overall water splitting activity. In comparison with reported literatures, such photocatalyst represents the excellent performance among all reported transition-metal oxides and/or transition-metal sulfides and is even superior to noble metal catalyst.
Funding Information
  • National Natural Science Foundation of China (22108214)

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