在基于氧的Pd2L4和Pd4L8协调中进行自我组装,相互锁定,相互转换和离子结合催化
Qiong-Yan Hong1, Bin Huang1, Meng-Xiang Wu1
1State Key Laboratory of Petroleum Molecular & Process Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China.
Nature communications
|March 14, 2025
概括
研究人员探索了基于氧的协调的溶剂介导的相互转换. 他们发现,溶剂控制着单体和互锁二元体的形成,揭示了组装机制的洞察力.
科学领域:
- 超分子化学 超分子化学
- 协调化学 协调化学
- 材料科学 材料科学 材料科学
背景情况:
- 自组装的协调,特别是Pd2L4型结构,经常表现出相互透.
- 控制子相互透的精确机制仍然不太清楚.
- 控制子组装和相互透对于开发先进的功能性材料至关重要.
研究的目的:
- 为了合成和表征基于诺的单体 (1) 和相互锁定的二极体 (2) 协调.
- 为了研究单体形和二元形之间的溶剂介导的相互转换.
- 阐明溶剂和离子在模板组装和相互透中的作用.
主要方法:
- 基于氧的协调子的合成.
- 单晶X射线衍射用于结构分析.
- 溶剂依赖的自我组装和相互转换研究.
- 阳离子结合和催化活性评估.
主要成果:
- 成功合成和分离了单体1和二元2.
- 展示了单体和二元之间的溶剂控制的相互转换.
- 确定特定的溶剂特性 (协调强度),驱动单体转为二元和二元转为单体的转换.
- 观察到化物离子模拟相互透,这表明子2在C-Cl键裂解中起着催化作用.
结论:
- 单体和二元协调之间的相互转换是由溶剂特性热力学驱动的.
- 溶剂选择对于控制自组装结果至关重要,使特定架构的隔离成为可能.
- 二次子表现出离子结合能力,并可能在离子模板反应中起到催化剂的作用.
相关概念视频
Protein Complex Assembly
10.5K
Proteins can form homomeric complexes with another unit of the same protein or heteromeric complexes with different types. Most protein complexes self-assemble spontaneously via ordered pathways, while some proteins need assembly factors that guide their proper assembly. Despite the crowded intracellular environment, proteins usually interact with their correct partners and form functional complexes.
Many viruses self-assemble into a fully functional unit using the infected host cell to...
Many viruses self-assemble into a fully functional unit using the infected host cell to...
10.5K
Pericyclic Reactions: Introduction
8.2K
Pericyclic reactions are organic reactions that occur via a concerted mechanism without generating any intermediates. The reactions proceed through the movement of electrons in a closed loop to form a cyclic transition state, where rearrangement of the σ and π bonds yields specific products.
Pericyclic reactions can be classified into three categories: electrocyclic reactions, cycloaddition reactions, and sigmatropic rearrangements. Electrocyclic reactions and sigmatropic...
Pericyclic reactions can be classified into three categories: electrocyclic reactions, cycloaddition reactions, and sigmatropic rearrangements. Electrocyclic reactions and sigmatropic...
8.2K
Aryldiazonium Salts to Azo Dyes: Diazo Coupling
2.9K
The reaction of weakly electrophilic aryldiazonium (also called arenediazonium) salts with highly activated aromatic compounds leads to the formation of products with an —N=N— link, called an azo linkage. This reaction, presented in Figure 1, is known as diazo coupling and occurs without the loss of the nitrogen atoms of the aryldiazonium salt. Highly activated aromatic compounds such as phenols or arylamines favor the diazo coupling reaction. The coupling generally occurs at the...
2.9K
Radical Reactivity: Overview
2.0K
Radicals, the highly reactive species, gain stability by undergoing three different reactions. The first reaction involves a radical-radical coupling, in which a radical combines with another radical, forming a spin‐paired molecule. The second reaction is between a radical and a spin‐paired molecule, generating a new radical and a new spin‐paired molecule. The third reaction is radical decomposition in a unimolecular reaction, forming a new radical and a spin‐paired...
2.0K
Oxidation of Phenols to Quinones
2.8K
In the presence of oxidizing agents, phenols are oxidized to quinones. Quinones can be easily reduced back to phenols using mild reducing agents. The electron-donating hydroxyl group enhances the reactivity of the aromatic ring, enabling oxidation of the ring even in the absence of an α hydrogen.
o-hydroxy phenols are oxidized to o-quinones and p-hydroxy phenols to p-quinones. Such redox reactions involve the transfer of two electrons and two protons. The reversible redox...
o-hydroxy phenols are oxidized to o-quinones and p-hydroxy phenols to p-quinones. Such redox reactions involve the transfer of two electrons and two protons. The reversible redox...
2.8K
Radical Chain-Growth Polymerization: Mechanism
2.4K
The radical chain-growth polymerization mechanism consists of three steps: initiation, propagation, and termination of polymerization. The polymerization initiates when a free radical generated from the radical initiator adds to the unsaturated bond in the monomer. The unpaired electron of the free radical and one π electron in the unsaturated bond creates a σ bond between the free radical and the monomer. As a result, the other π electron in the unsaturated bond converts this...
2.4K


