通过激发状态的分子内质子转移驱动交叉系统在二维共价有机框架中产生无金属单片氧气
Junyi Qiu1, Chang Cheng1, Hermenegildo García2
1Laboratory of Solar Fuel, Faculty of Materials Science and Chemistry, China University of Geosciences, 68 Jincheng Street, Wuhan, 430078, P.R. China.
Angewandte Chemie (International ed. in English)
|October 14, 2025
概括
没有金属的兴奋状态分子内质子转移 (ESIPT) 策略增强单片氧 (O2) 生产. 两维共价有机框架 (2D COF) 能够稳定ESIPT过渡,促进系统间交叉 (ISC) 在光催化中高效的O2生成.
科学领域:
- 光催化作用的光催化
- 材料科学 材料科学 材料科学
- 有机化学 有机化学
背景情况:
- 单片氧 (O2) 对于光动力学疗法和有机合成至关重要.
- 传统方法使用金属敏化剂,带来生物相容性和可扩展性问题.
- 需要无金属的方法来实现可持续和高效的O2发电.
研究的目的:
- 开发一种无金属的策略,以提高单片氧 (1O2) 的生产.
- 研究激发状态分子内质子转移 (ESIPT) 在O2生成中的作用.
- 为了比较1D聚合物和2D共价有机框架 (COF) 在ESIPT介导的O2合成中的性能.
主要方法:
- 使用ESIPT合成和描述1D聚合物和2DCOF.
- 时间解析的光谱研究,以监测ESIPT和系统间交叉 (ISC) 动态.
- 热力学分析和边界分子轨道计算以阐明ISC机制.
主要成果:
- 二维的COF表现出稳定的ESIPT过渡,导致持久的元稳定状态.
- 与1D聚合物相比,2DCOF中的这种稳定状态促进了增强的系统间交叉 (ISC).
- 2D COF 中的 ESIPT 触发 ISC,显著提升单片氧 (O2) 生成.
结论:
- 基于二维COF的ESIPT转换为高效的O2生成提供了优越的无金属途径.
- 在二维COF中稳定定体转换是提高ISC效率的关键.
- 这项工作扩大了ESIPT在光催化中的应用,特别是促进O2的生产.
相关概念视频
Metal-Ligand Bonds
24.0K
The hemoglobin in the blood, the chlorophyll in green plants, vitamin B-12, and the catalyst used in the manufacture of polyethylene all contain coordination compounds. Ions of the metals, especially the transition metals, are likely to form complexes.
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
In these complexes, transition metals form coordinate covalent bonds, a kind of Lewis acid-base interaction in which both of the electrons in the bond are contributed by a donor (Lewis base) to an electron acceptor (Lewis acid). The Lewis acid in...
24.0K
Bonding in Metals
51.8K
Metallic bonds are formed between two metal atoms. A simplified model to describe metallic bonding has been developed by Paul Drüde called the “Electron Sea Model”.
51.8K
Oxidation and Reduction of Organic Molecules
9.1K
Energy production within a cell involves many coordinated chemical pathways. Most of these pathways are combinations of oxidation and reduction reactions, which occur at the same time. An oxidation reaction strips an electron from an atom in a compound, and the addition of this electron to another compound is a reduction reaction. Because oxidation and reduction usually occur together, these pairs of reactions are called redox reactions.
The removal of an electron from a molecule, results in a...
The removal of an electron from a molecule, results in a...
9.1K
Lewis Structures of Molecular Compounds and Polyatomic Ions
44.6K
To draw Lewis structures for complicated molecules and molecular ions, it is helpful to follow a step-by-step procedure as outlined:
44.6K
Oxidative Cleavage of Alkenes: Ozonolysis
12.7K
In ozonolysis, ozone is used to cleave a carbon–carbon double bond to form aldehydes and ketones, or carboxylic acids, depending on the work-up.
Ozone is a symmetrical bent molecule stabilized by a resonance structure.
Ozone is a symmetrical bent molecule stabilized by a resonance structure.
12.7K
Resonance and Hybrid Structures
25.1K
According to the theory of resonance, if two or more Lewis structures with the same arrangement of atoms can be written for a molecule, ion, or radical, the actual distribution of electrons is an average of that shown by the various Lewis structures.
Resonance Structures and Resonance Hybrids
The Lewis structure of a nitrite anion (NO2−) may actually be drawn in two different ways, distinguished by the locations of the N–O and N=O bonds.
Resonance Structures and Resonance Hybrids
The Lewis structure of a nitrite anion (NO2−) may actually be drawn in two different ways, distinguished by the locations of the N–O and N=O bonds.
25.1K


