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Supramolecular Self-Assembly of Nitrogen-Deficient Ag/g-C3N4 Nanofiber Films with Enhanced Charge Transfer Dynamics for Efficient Visible-Light Photocatalytic Activity
ACS Applied Materials & Interfaces ( IF 9.5 ) Pub Date : 2021-10-13 , DOI: 10.1021/acsami.1c15321
Lin Chen 1 , Sudong Yang 1, 2 , Wensheng Qi 1 , Qian Zhang 1 , Jie Zhu 1 , Peng Zhao 1
Affiliation  

Molecular self-assembly of organic molecules through noncovalent interactions is a powerful strategy for designing functional materials. Herein, we fabricated a novel free-standing Ag/g-C3N4 nanofiber (Ag/CNNF) film via a water-based molecular engineering approach followed by pyrolysis using a cyanuric acid–melamine complex as the precursor. Uniform dispersion of plasmonic Ag nanoparticles and incorporation of nitrogen vacancies were synchronously introduced into the 3D highly interconnected porous CNNF framework. The resulting Ag/CNNF film with multilevel interlayer spacing distributions significantly expedited more sufficient charge transfer dynamics not only at Schottky junction sites but also throughout hierarchical CN by exciton dissociation. Benefiting from the synergistic enhancement in visible light harvesting capability and steered charge carrier transfer in a longitudinal direction, the Ag/CNNF film presented remarkably boosted photocatalytic ability both for hydrogen production and tetracycline degradation. The optimal Ag/CNNF-2 film exhibited a prominent photocatalytic hydrogen evolution rate of 1240 μmol g–1 h–1 without the Pt co-catalyst under visible light illumination, which was 10.3 times as high as that of bulk g-C3N4. Significantly, 1D Ag/g-C3N4 nanofibers self-assembled into an ordered and macroscopic film, which was more favorable in practical applications owing to good reusability and high processability. This work paved the way for the facile preparation of supramolecular self-assembled CN-based film photocatalysts.

中文翻译:

具有增强的电荷转移动力学的缺氮 Ag/g-C3N4 纳米纤维膜的超分子自组装以实现有效的可见光光催化活性

通过非共价相互作用进行有机分子的分子自组装是设计功能材料的有力策略。在此,我们制造了一种新型的独立式 Ag/gC 3 N 4通过水基分子工程方法制备纳米纤维(Ag/CNNF)薄膜,然后使用氰尿酸-三聚氰胺复合物作为前体进行热解。等离子体银纳米粒子的均匀分散和氮空位的结合被同步引入到 3D 高度互连的多孔 CNNF 框架中。由此产生的具有多级层间距分布的 Ag/CNNF 膜不仅在肖特基结位点而且通过激子解离在整个分级 CN 中显着加速了更充分的电荷转移动力学。受益于可见光捕获能力和纵向载流子转移的协同增强,Ag/CNNF 薄膜在产氢和四环素降解方面均表现出显着增强的光催化能力。–1 h –1在可见光照射下没有 Pt 助催化剂,是块状 gC 3 N 4 的10.3 倍。值得注意的是,一维Ag/gC 3 N 4纳米纤维自组装成有序且宏观的薄膜,由于良好的可重复使用性和高加工性,这在实际应用中更有利。该工作为简单制备超分子自组装CN基薄膜光催化剂铺平了道路。
更新日期:2021-10-27
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