Bifunctional Hydrogen Production and Storage on 0D–1D Heterojunction of Cd0.5Zn0.5S@Halloysites

Abstract Development of efficient solar‐driven hydrogen (H 2 ) evolution and H 2 storage materials is challenging. Sulfide nanocatalysts show large potential for H 2 production, but suffer from the drawbacks of inefficient charge separation, serious photocorrosion, and easy agglomeration. Herein, a 0D–1D satellite‐core ethylenediaminetetraacetic acid (EDTA)‐bridged Cd 0.5 Zn 0.5 S@halloysite nanotubes tertiary structure is designed via facile in situ assembly, which settles all the above‐mentioned issues and achieves exceptional and stable photocatalytic H 2 evolution and storage. Significantly, EDTA grafted on halloysites as the hole (h + ) traps steers the photogenerated h + and electrons (e − ) from Cd 0.5 Zn 0.5 S separately to halloysites and outer surface Pt sites, achieving efficient directional separation between h + and e − and inhibiting the h + ‐dominated photocorrosion occurring on Cd 0.5 Zn 0.5 S. Benefiting from these advantages, the hierarchy shows an unprecedented photocatalytic H 2 evolution rate of 25.67 mmol g −1 h −1 with a recording apparent quantum efficiency of 32.29% at λ = 420 nm, which is seven‐fold that of Cd 0.5 Zn 0.5 S. Meanwhile, an H 2 adsorption capacity of 0.042% is achieved with the room temperature of 25 °C and pressure of 2.65 MPa. This work provides a new perspective into designing hierarchical structure for H 2 evolution, and proposes an integration concept for H 2 evolution and storage.