Constructing Robust Interfacial Chemical Bond Enhanced Charge Transfer in S‐Scheme 3D/2D Heterojunction for CO₂ Photoreduction

A stable ZnTe@Cs 3 Sb 2 I 9 catalyst with 3D/2D‐hollow‐composite structure is constructed for CO 2 photocatalytic reduction via the in situ growth of Cs 3 Sb 2 I 9 nanosheets on hollow ZnTe microspheres using lattice matching. The formed Tellurium‐Antimony (Te─Sb) bonds improved the poor contact at the heterojunction interface, effectively promoted charge separation, and successfully suppressed photocorrosion. The unique core‐shell structure not only strengthens light absorption but also improves CO 2 adsorption capacity. Consequently, the S‐scheme heterojunction with the synergistic effect of chemical bonds and 3D/2D‐hollow‐composite structure significantly enhances photocatalytic performance. The ZnTe@Cs 3 Sb 2 I 9 photocatalyst offers a CO selectivity of 90.5%, which is higher than that of pure ZnTe (22.9%) and Cs 3 Sb 2 I 9 (56.9%). This structure holds great promise for practical applications in CO 2 photocatalytic reduction.