Synthesis of Carbon Nitride Polymorphs by Sacrificial Template Method: Correlation between Physicochemical Properties and Photocatalytic Performance.

Abstract

Carbon nitride compounds (CNCs) in the form of graphitic carbon nitride (g-C3N4) and poly(heptazine imide) were synthesized using different metal chloride salts (MClx), i.e., NaCl, KCl and CaCl2, as sacrificial templates and by varying the MClx to melamine molar ratios. A systematic study of their photocatalytic activity for H2 production in relation to the physicochemical, morphological, and optical properties was carried out. Each sample was tested achieving the highest hydrogen evolution rates of about 7660 µmol g-1 h-1, 5380 µmol g-1 h-1 and 3140 µmol g-1 h-1 using CaCl2, KCl, and NaCl, respectively. This work demonstrates how the synthesis of CNCs with different MClx leads to the production of high-performance photocatalysts due to a combination of factors as the formation of vacancies or cyano groups, a shift in the optical threshold and tuning of micro(nano)structure. The results demonstrate that, when CaCl2 is used as a sacrificial template, porous and exfoliated g-C3N4 nanosheets are formed leading to hydrogen productions which outperform most of the previously reported g-C3N4 prepared using a single synthetic step.