Graphdiyne(CnH2n‐2)‐Based NiCo LDH – Graphdiyne – CuI Double S‐Scheme Heterojunction For Efficient Photocatalytic Hydrogen Production**

Abstract Graphdiyne (GDY), a new two‐dimensional carbon isomer material, has received much attention due to its excellent properties, but has been less applied in the field of photocatalytic hydrogen production. Different from the conventional method, in this paper, GDY−CuI binary heterojunctions are prepared by the one‐pot method, and then GDY−CuI is combined with different morphologies of NiCoLDH (NiCoLDH‐F and NiCoLDH‐R; LDH=layered double hydroxide) through morphology modulation to form NiCoLDH−CuI−GDY double S‐scheme heterojunction catalysts. On the one hand, NiCoLDH could provide sufficient anchor sites for GDY−CuI, which is conducive to the separation and transport of electrons at the contact interface and provides abundant reaction sites for the hydrogen precipitation reaction. NiCoLDH in the form of nanorods is more stable and provides more active sites for hydrogen precipitation than NiCoLDH in the form of nanoflowers. On the other hand, the construction of double S‐scheme heterojunctions can promote electron transfer and exhibit strong redox ability in photocatalytic reactions, so the hydrogen precipitation activity is enhanced. Most importantly, both NiCoLDH‐F−CuI−GDY (12.09 μmol ⋅ h−1) and NiCoLDH‐R−CuI−GDY (13.47 μmol ⋅ h−1) exhibited excellent hydrogen precipitation activity. This experiment provides a new strategy for the construction of an efficient and environmentally friendly multicatalytic system.