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Atomic symmetry alteration in carbon nitride to modulate charge distribution for efficient photocatalysis
Journal of Catalysis ( IF 6.5 ) Pub Date : 2023-01-04 , DOI: 10.1016/j.jcat.2023.01.003
Minhua Ai , Lun Pan , Ying Chen , Chengxiang Shi , Zhen-Feng Huang , Xiangwen Zhang , Ji-Jun Zou

The periodical distribution of N and C atoms in the carbon nitride skeleton results in intrinsically insufficient 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-π* 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 production and RhB degradation than the pristine one (CN-0CYS), respectively.



中文翻译:

改变氮化碳中的原子对称性以调节电荷分布以实现高效光催化

氮化碳骨架中N和C原子的周期性分布导致本质上光吸收不足和严重的载流子复合。在此,开发了一种有效的两步胱氨酸介导策略来改变 C 3 N 4的结构对称性通过引入烷基和氮空位。实验分析和理论计算证实,烷基和氮空位的形成可以调节能带结构,激活n-π*电子跃迁。特别是,CN-25CYS中的电荷密度重新分布,氧化还原位点在空间上分离,有效抑制了光生电荷复合。因此,变形的氮化碳 (CN-25CYS) 在制氢和 RhB 降解方面的光反应速率分别比原始氮化碳 (CN-0CYS) 高 9.6 倍和 15.6 倍。

更新日期:2023-01-07
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