光活性共价有机框架中的坚固链接在恶劣条件下能够实现有效的光催化反应
Jia-Rui Wang1, Kepeng Song1, Tian-Xiang Luan1
1School of Chemistry and Chemical Engineering, Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion, Science Center for Material Creation and Energy Conversion, Shandong University, No. 27 Shanda South Road, Ji'nan, 250100, PR China.
Nature communications
|February 10, 2024
概括
研究人员开发了强大的素链接共价有机框架 (COF) 用于苛刻的光催化. 这些稳定的COF在具有挑战性的反应中表现出增强的活性和可回收性,表现优于传统的因胺结合的COF.
科学领域:
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
- 有机化学 有机化学
背景情况:
- 开发稳定的异质光催化剂以适应恶劣的条件至关重要,但具有挑战性.
- 共价有机框架 (COF) 提供可调节的特性,但在苛刻的反应环境下往往缺乏稳定性.
研究的目的:
- 为在恶劣条件下的反应合成和表征新的,强大的共价有机框架 (COF),增强稳定性和光催化活性.
- 调查与其 imine-linked对应物相比,林结合COF在要求高的光催化应用中的性能.
主要方法:
- 合成了三烯胺结合的共价有机框架 (COFs) 通过将 imine 链接转化为类组,生成 TFPA-TAPT-COF-Q 和 TFPA-TPB-COF-Q.
- 通过可回收反应评估合成的COF的光催化活性和稳定性,包括有机酸的氧化脱碳化和胺合.
- 在强烈的氧化条件下对氧化生产中,评估了与素相关的COF的效率和长期可用性.
主要成果:
- 成功构建了两种光敏诺林结合的COF (TFPA-TAPT-COF-Q和TFPA-TPB-COF-Q) 的稳定性得到改善.
- 与 imine-linked COF相比,在有机酸和合反应中表现出更高的 photocatalytic 活性和可回收性.
- 在恶劣的氧化条件下,通过使用oline-linked COFs实现了高效率 (11831.6 μmol·g-1·h-1) 和长期可回收,用于生产过氧化.
结论:
- 增强光活性COF的结合稳定性,特别是通过将imine转化为林组,是开发稳定的异质催化剂的高效策略.
- 诺林结合的COF是光催化应用的有希望的候选物,在恶劣的环境条件下需要高稳定性和活性.
- 开发的COF为高效和可持续的光催化过程提供了可行的途径,包括H2O2生产.
相关概念视频
01:12Cycloaddition Reactions: MO Requirements for Photochemical Activation
2.1K
Some cycloaddition reactions are activated by heat, while others are initiated by light. For example, a [2 + 2] cycloaddition between two ethylene molecules occurs only in the presence of light. It is photochemically allowed but thermally forbidden.
2.1K
01:26Photochemical Electrocyclic Reactions: Stereochemistry
1.8K
The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
Selection Rules: Photochemical Activation
Selection Rules: Photochemical Activation
1.8K
01:26Thermal and Photochemical Electrocyclic Reactions: Overview
2.3K
Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
2.3K
01:29The Photochemical Reaction Center
4.1K
Reaction centers are pigment-protein complexes that initiate energy conversion from photons to chemical entities. Therefore, photochemical reaction center is a more appropriate term that describes these complexes. The Nobel laureates Robert Emerson and William Arnold provided the first experimental evidence of photochemical reaction centers by demonstrating the participation of nearly 2,500 chlorophyll molecules for the release of just one molecule of oxygen. Despite thousands of photosynthetic...
4.1K