光化学
噻吩
光催化
分子内力
介孔材料
材料科学
接受者
氮化碳
离域电子
催化作用
化学
有机化学
凝聚态物理
物理
作者
Zongzhao Sun,Yabin Jiang,Lei Zeng,Limin Huang
出处
期刊:Chemsuschem
[Wiley]
日期:2019-03-22
卷期号:12 (7): 1325-1333
被引量:57
标识
DOI:10.1002/cssc.201802890
摘要
Abstract Inspired by donor–acceptor (D–A) polymers in organic solar cell and the extended conjugation effect, a conceptual design of D–π–A‐type mesoporous carbon nitride with benzene or thiophene as a π‐spacer is proposed as an efficient photocatalyst for hydrogen evolution. The photocatalyst was successfully synthesized by a one‐pot thermopolymerization based on nucleophilic substitution and a Schiff‐base chemical reaction. On the molecular level, the insertion of an in‐plane benzene as a π‐spacer by forming covalent bonds C=N (acceptor) and C−N (donor) interrupts the continuity of tri‐ s ‐triazine units and maintains the intrinsic π–π conjugated electronic system. Synchronously, the enlarged electron delocalization and the intramolecular charge transfer induced by polarization provide force‐directed migration of electrons, leading to boosted optical absorption capability and enhanced photogenerated carrier separation. With the synergistic effects of the mesoporous structure and excellent optical and electronic properties, a fivefold increase in the H 2 evolution rate compared with that of pristine g‐C 3 N 4 was achieved with robust performance. In addition, other simple aromatic heterocyclic compounds (e.g., pyridine, thiophene and furan)‐based D–π–A structures with a higher hydrogen evolution rate (up to sevenfold increase) were also explored to broaden the application for the design of novel photocatalysts.
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