Salt-melt synthesis of poly(heptazine imide) in binary alkali metal bromides for enhanced visible-light photocatalytic hydrogen production
Yaxuan Jin , Dandan Zheng , Zhongpu Fang , Zhiming Pan , Sibo Wang , Yidong Hou , Oleksandr Savateev , Yongfan Zhang , Guigang Zhang
Interdisciplinary Materials ›› 2024, Vol. 3 ›› Issue (3) : 389 -399.
Salt-melt synthesis of poly(heptazine imide) in binary alkali metal bromides for enhanced visible-light photocatalytic hydrogen production
Poly(heptazine imide) (PHI), a semicrystalline version of carbon nitride photocatalyst based on heptazine units, has gained significant attention for solar H2 production benefiting from its advantages including molecular synthetic versatility, excellent physicochemical stability and suitable energy band structure to capture visible photons. Typically, PHI is obtained in saltmelt synthesis in the presence of alkali metal chlorides. Herein, we examined the role of binary alkali metal bromides (LiBr/NaBr) with diverse compositions and melting points to rationally modulate the polymerization process, structure, and properties of PHI. Solid characterizations revealed that semicrystalline PHI with a condensed π-conjugated system and rapid charge separation rates were obtained in the presence of LiBr/NaBr. Accordingly, the apparent quantum yield of hydrogen using the optimized PHI reaches up to 62.3% at 420 nm. The density functional theory calculation shows that the dehydrogenation of the ethylene glycol has a lower energy barrier than the dehydrogenation of the other alcohols from the thermodynamic point of view. This study holds great promise for rational modulation of the structure and properties of conjugated polymeric materials.
crystallinity / hydrogen evolution / photocatalysis / poly(heptazine imide) / salt-melt synthesis
2024 The Authors. Interdisciplinary Materials published by Wuhan University of Technology and John Wiley & Sons Australia, Ltd.
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