2D/1D MoS₂/TiO₂ Heterostructure Photocatalyst with a Switchable CO₂ Reduction Product

Abstract Regulating the transfer pathway of charge carriers in heterostructure photocatalysts is of great importance for selective CO₂ photoreduction. Herein, the charge transfer pathway and in turn the redox potential succeeded to regulate in 2D MoS₂/1D TiO₂ heterostructure by varying the light wavelength range. Several in situ measurements and experiments confirm that charge transfer follows either an S‐scheme mechanism under simulated solar irradiation or a heterojunction approach under visible light illumination, elucidating the switchable property of the MoS₂/TiO₂ heterostructure. Replacing the simulated sunlight irradiation with the visible light illumination switches the photocatalytic CO₂ reduction product from CO to CH_4. ¹³CO₂ isotope labeling confirms that CO₂ is the source of carbon for CH₄ and CO products. The photoelectrochemical H₂ generation further supports the switching property of MoS₂/TiO₂. Unlike previous studies, density functional theory calculations are used to investigate the band structure of Van der Waals MoS₂/TiO₂ S scheme after contact, allowing to propose accurate charge transfer pathways, in which the theoretical results are well matched with the experimental results. This work opens the opportunity to develop photocatalysts with switchable charge transport and tunable redox potential for selective artificial photosynthesis.