期刊
CHEMISTRY-AN ASIAN JOURNAL
卷 13, 期 20, 页码 3073-3083出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/asia.201801083
关键词
electronic structure; hydrogen; photocatalysis; nitrides; nitrogen heterocycles
资金
- National Natural Science Foundation of China [21773074, 21273080]
In this study, a photocatalyst with a distorted skeleton and synthesized by grafting triamterene onto graphitic carbon nitride (g-C3N4) frameworks was prepared. The pteridine ring of the triamterene-based nitrogen-enriched organic structure functions as a trapped electron site owing to its inductive effect. The benzene ring in triamterene plays an important role in the even dispersion of electrons by a conjugative effect. Redistribution of the intramolecular electronic potential is caused by a synergistic effect between the pteridine and benzene rings of triamterene and promotes separation and migration of the photoinduced charge carriers. After coupling with triamterene, the electrons of g-C3N4 are relocated; that is, the intrinsic electronic and band structures of g-C3N4 are effectively modulated. The modified polymeric photocatalyst shows a high photocatalytic H-2 evolution rate of 157.5molh(-1), a value that is 4.3 times higher than the H-2 evolution rate of pristine g-C3N4 (36.8molh(-1)), with an apparent quantum efficiency of 9.7% at =450nm. The incorporation of triamterene into the g-C3N4 frameworks significantly expands its -delocalized system by redistribution of the electronic potential, expands the visible-light absorption range, and effectively promotes the separation and migration of photoinduced charge carriers. This strategy may provide a reference for promoting charge separation of g-C3N4 through redistribution of the electronic potential and for synthesizing novel carbon nitride based semiconductors for efficient solar energy conversion into hydrogen.
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