Enhanced photocatalytic hydrogen production activity of highly crystalline carbon nitride synthesized by hydrochloric acid treatment

Crystalline carbon nitride(CCN)prepared by a molten-salt method is attracting increased attention because of its promising properties and excellent photocatalytic activity.In this work,we further improve the crystallinity of CCN through synthesis by the molten-salt method under the action of aqueous hydrochloric acid(HCl)solution.Our results showed that the crystallinity of the as-prepared samples increased with increasing HCl concentration and reached the maximum value at 0.1 mol L^-1.This can be attributed to the removal of some potassium ions(K+)from the terminal amino groups of CCN by the aqueous HCl solution,which results in a release of the polymerization sites.As a result,the crystallinity of the as-prepared samples further increased.Moreover,the obtained 0.1 highly crystalline carbon nitride(0.1HCCN;treated with 0.1 mol L^-1 aqueous HCl solution)exhibited an excellent photocatalytic hydrogen evolution of 683.54μmol h^-1 g^-1 and a quantum efficiency of 6.6%at 420 nm with triethanolamine as the sacrificial agent.This photocatalytic hydrogen evolution was 2 and 10 times higher than those of CCN and bulk carbon nitride,respectively.The enhanced photocatalytic activity was attributed to the improved crystallinity and intercalation of K+into the xHCCN interlayer.The improved crystallinity can decrease the number of surface defects and hydrogen bonds in the as-prepared sample,thereby increasing the mobility of the photoinduced carriers and reducing the recombination sites of the electron-hole pairs.The K+intercalated into the xHCCN interlayer also promoted the transfer of the photoinduced electrons because these ions can increase the electronic delocalization and extend theπ-conjugated systems.This study may provide new insights into the further development of the molten-salt method.