Mesoporous Polymeric Cyanamide-Triazole-Heptazine Photocatalysts for Highly-Efficient Water Splitting
Mesoporous Polymeric Cyanamide-Triazole-Heptazine Photocatalysts for Highly-Efficient Water Splitting
复制标题
用于高效水分解的介孔聚合物氰胺-三唑-庚嗪光催化剂
DOI：
10.1002/smll.202003162
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发表时间：
2020-08-12
期刊：
影响因子：
13.3
通讯作者：
Wang, Bo
中科院分区：
文献类型：
--
作者：
Wu, Chongbei;Yu, Guanhang;Wang, Bo
共轭聚合物由于其简单的合成和可调节的带隙，是用于水还原/氧化的有前途的光收集器。在本文中，首先将氰胺和三唑官能团引入基于七嗪的碳氮化物（CN）聚合物中，通过增加CN骨架中的氰胺/三唑单元的量，得到具有不同组成的介孔共轭氰胺-三唑-七嗪聚合物（CTHP）。改变CTHP的组成可以调节其电子结构、介孔形貌和氧化还原能，从而显著提高其在可见光照射下的光催化性能。在400 nm处，H（2）的释放速率为12723 μ mol·h（-1）·g（-1），表观量子产率为11.97%。同时，优化后的光催化剂的O（2）释放速率为221 μ mol·h（-1）·g（-1），是CN光催化剂的9.6倍，是已报道的CN基双功能光催化剂中最高的。本工作为功能高分子光催化剂的合理设计提供了一种有效的分子工程方法。
Conjugated polymers are promising light harvesters for water reduction/oxidation due to their simple synthesis and adjustable bandgap. Herein, both cyanamide and triazole functional groups are first incorporated into a heptazine-based carbon nitride (CN) polymer, resulting in a mesoporous conjugated cyanamide-triazole-heptazine polymer (CTHP) with different compositions by increasing the quantity of cyanamide/triazole units in the CN backbone. Varying the compositions of CTHP modulates its electronic structures, mesoporous morphologies, and redox energies, resulting in a significantly improved photocatalytic performance for both H(2)and O(2)evolution under visible light irradiation. A remarkable H(2)evolution rate of 12723 mu mol h(-1)g(-1)is observed, resulting in a high apparent quantum yield of 11.97% at 400 nm. In parallel, the optimized photocatalyst also exhibits an O(2)evolution rate of 221 mu mol h(-1) g(-1), 9.6 times higher than the CN counterpart, with the value being the highest among the reported CN-based bifunctional photocatalysts. This work provides an efficient molecular engineering approach for the rational design of functional polymeric photocatalysts.