Abstract
Producing green hydrogen by photoelectrocatalytic water splitting is one of the most promising approaches to conversion of renewable energy to chemical energy, which is restricted by the unsuitable energy barrier between the conduction band of the semiconductor and the H+/H2 level as well as the unsuitable binding energy of active sites with the intermediates in hydrogen evolution reaction. Herein, we rationally construct an n+p-Si/Ti/WO3@RuSe2 heterostructured photocatalyst, which significantly improves the photovoltage and photocurrent by charge redistribution between p-Si and heterostructured WO3@RuSe2. The representative n+p-Si/Ti/WO3@RuSe2 exhibits a photovoltage of 0.54 VRHE with a high short-circuit photocurrent density of −36 mA cm−2 and solar-to-hydrogen conversion efficiency of 9.43%, which is much higher than that of n+p-Si/Ti (0.45 VRHE, −0.22 mA cm−2, 0.015%). The characterizations and density functional theory calculations reveal that the heterostructured interface moves the d-band center of WO3@RuSe2 (−0.699 eV) to the Fermi level through the multistaged charge redistribution, thus reducing the barrier between the conduction band of p-Si and H+/H2 level as well as improving the charge separation efficiency.
Published Version
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