通过调节共价有机框架中的不和键,为太阳能H2O2生产提供明确的氧气减少途径
Jie-Yu Yue1, Zi-Xian Pan1, Yan Guo1
1Key Laboratory of Molecular and Nano Probes, Ministry of Education, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University Jinan 250014 P. R. China yuejieyu@sdnu.edu.cn yangpeng@sdnu.edu.cn.
Chemical science
|July 9, 2025
概括
研究人员通过改变不和键来精确控制共价有机框架 (COF) 中的两电子氧降解反应 (2e-ORR) 路径. 这一突破使得高效的光催化过氧化 (H2O2) 产生使用工程COFs.
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:
- 通过双电子氧降解反应 (2e-ORR) 产生光催化过氧化 (H2O2) 是一种可持续的过程.
- 控制特定的2e-ORR路径 (一步或两步) 仍然是材料设计中的一个重大挑战.
研究的目的:
- 为了证明2e-ORR途径在共价有机框架 (COF) 中的精确调制.
- 研究不和键在指导H2O2生产的2e-ORR机制中的作用.
主要方法:
- 同结构共价有机框架 (COF) 的合成,具有不同的不和键 (基与基).
- 对COF的表征和对其光催化H2O2生成性能的评估.
- 理论计算以阐明路径调制的机制.
主要成果:
- 含有基因的TY-COF倾向于两步2e-ORR路线,而含有基因的TE-COF则遵循了一步路线.
- 在没有牺牲剂的情况下,TY-COF和TE-COF实现了高H2O2生产率,分别为6455和4804μmol g-1 h-1,没有牺牲剂.
- 不和键的修改改变了电子孔分布,并重组了催化中心,导致ORR路径分歧.
结论:
- 在COF中,不和债券控制为精确调节2e-ORR路径提供了一种新的策略.
- 工程化COF,包括独立的膜,可以有效地驱动H2O2光合作用.
- 这项工作为设计用于选择性化学转换的先进催化剂提供了宝贵的见解.
相关概念视频
Oxidation and Reduction of Organic Molecules
7.7K
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...
7.7K
Oxygenic Photosynthesis
203
Oxygenic photosynthesis is a fundamental process in which light energy is harnessed to drive the oxidation of water, leading to the production of molecular oxygen (O₂), adenosine triphosphate (ATP), and nicotinamide adenine dinucleotide phosphate (NADPH). This process is essential for sustaining aerobic life on Earth and is primarily carried out by cyanobacteria, algae, and plants. The core of oxygenic photosynthesis lies in the thylakoid membranes, where chlorophyll pigments facilitate...
203
The Z-Scheme of Electron Transport in Photosynthesis
10.6K
The light reactions of photosynthesis assume a linear flow of electrons from water to NADP+. During this process, light energy drives the splitting of water molecules to produce oxygen. However, oxidation of water molecules is a thermodynamically unfavorable reaction and requires a strong oxidizing agent. This is accomplished by the first product of light reactions: oxidized P680 (or P680+), the most powerful oxidizing agent known in biology. The oxidized P680 that acquires an electron from the...
10.6K
Oxidative Cleavage of Alkenes: Ozonolysis
11.2K
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.
11.2K
Oxidation of Alkenes: Syn Dihydroxylation with Osmium Tetraoxide
10.8K
Alkenes are converted to 1,2-diols or glycols through a process called dihydroxylation. It involves the addition of two hydroxyl groups across the double bond with two different stereochemical approaches, namely anti and syn. Dihydroxylation using osmium tetroxide progresses with syn stereochemistry.
10.8K
Phase I Oxidative Reactions: Overview
383
Phase I biotransformation, or functionalization, is a crucial chemical process that converts drugs and other xenobiotics into more water-soluble forms, facilitating expulsion from the body. It involves oxidative, reductive, and hydrolytic reactions that add or unveil polar functional groups on lipophilic substrates. Key players in phase I reactions are the mixed-function oxidases. Situated in liver cell microsomes, these enzymes predominantly carry out drug metabolism. They require molecular...
383


