Atomic symmetry alteration in carbon nitride to modulate charge distribution for efficient photocatalysis

The periodical distribution of N and C atoms in the carbon nitride skeleton results in intrinsically insuf-ficient light absorption and serious carrier recombination. Herein, an efficient two-step cystine-mediated strategy was developed to alter the structure symmetry of C3N4 via the introduction of alkyl groups and nitrogen vacancies. The experimental analysis and theoretical calculation confirm that the formation of alkyl groups and nitrogen vacancies can modulate band structure and activate n -1t* electron transition. Especially, the charge density in CN-25CYS is redistributed with spatial separation of oxidation and reduction sites, suppressing photogenerated charge recombination effectively. Therefore, the distorted carbon nitride (CN-25CYS) exhibits 9.6-times and 15.6-times higher photoreaction rates in hydrogen pro-duction and RhB degradation than the pristine one (CN-0CYS), respectively.(c) 2023 Elsevier Inc. All rights reserved.

Automated summary

An efficient two-step cystine-mediated strategy was developed to alter the structure symmetry of C3N4, leading to the redistribution of N and C atoms and improved light absorption and carrier recombination. Experimental analysis and theoretical calculation show that the introduction of alkyl groups and nitrogen vacancies can modulate the band structure and activate electron transition, resulting in effective suppression of charge recombination. The distorted carbon nitride exhibits significantly higher photoreaction rates in hydrogen production and RhB degradation compared to the pristine one.