Strategy of Graphdiyne (g−CnH2n‐2 ) Preparation Coupling with the Flower‐Like NiAl‐LDH Heterojunctions for Efficient Photocatalytic Hydrogen Evolution**

Abstract Graphdiyne (g−C n H 2n‐2 ), a novel two‐dimension carbon allotrope material composed of a sp‐ and sp 2 ‐hybrid carbon network, has been widely explored since it was synthesized for the first time by Li's group in 2010. A series distinct and excellent properties bestow graphdiyne excellent performance in many fields. Here, an innovative progress for preparing graphdiyne by using Cu + contained material as catalyst is reported and the composite CuI‐GD is coupled with flower‐like NiAl‐LDH to produce H 2 from photocatalytic water splitting. The results of FTIR and Raman spectroscopy together reveal that graphdiyne nanosheets are synthesized successfully by employing a cross‐coupling method. Photocatalytic hydrogen evolution performance shows that the hydrogen production activity of CuI‐GD/NiAl‐LDH has a 15‐ and 216‐fold enhancement compared with CuI‐GD and NiAl‐LDH, respectively. A series of characterizations are carried out to expound the underlying reasons in the enhancement of the photocatalytic hydrogen production performance of CuI‐GD/NiAl‐LDH. Meanwhile, a possible mechanism for the photocatalytic hydrogen evolution process was proposed to understand the interaction among these materials.