基于多氧甲酸盐的高核度金属有机框架用于C-C键的光催化氧化裂变
Qixin Zhao1, Yang Zeng1, Zhiqiang Jiang1
1State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Chemistry and Chemical Engineering, Donghua University, Shanghai, 201620, P. R. China.
Angewandte Chemie (International ed. in English)
|December 9, 2024
概括
研究人员创建了新型的高核度聚氧金属 (POM) 集群,并使用它们来构建迄今为止最高核度的POM衍生金属有机框架 (MOF). 这些POM-MOF显示出对绿色催化有希望,特别是在木质素降解中.
科学领域:
- 无机化学 无机化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 高核性聚氧金属 (POM) 集群是金属有机框架 (MOF) 的有价值的构建块,因为它们的连接性和多重金属中心.
- 现有的基于POM的MOF通常缺乏高级功能应用所需的高核度.
- 开发合成新型POM集群并将其纳入MOF的策略对于创建先进材料至关重要.
研究的目的:
- 制定一个逐步的增长战略,用于合成新的高核性多氧化态集群.
- 使用这些POM集群作为节点构建新的金属有机框架 (MOF).
- 研究这些POM-MOF在光催化应用中的潜力,特别是素模型裂变.
主要方法:
- 环状[P8W48O184]40-前体的逐步合成,产生半封闭的{W58}和完全封闭的{W64}多氧化态.
- 在现场构建基于铜三醇-酸 (HL) 复合物的MOF,其中包括{W58}和{W64}集群.
- 调整反应条件,主要是溶液的pH值,以控制POM形成和MOF合成的联体质子.
- 对MOF结构的表征和对素模型氧化裂变的光催化活性的评估.
主要成果:
- 成功合成了两种新的高核性多氧化物状态,W58和W64.
- 两种新的POM衍生MOF,HNPOMOF-1 ({Cu11(HL) 9W58}) 和HNPOMOF-2 ({Cu9(HL) 9W64}),显示迄今为止最高的核度,被制造出来.
- HNPOMOF-1具有3D框架,具有类似子的空洞,而HNPOMOF-2则形成2D层,可以剥离成纳米薄膜 (HNPOMOF-2NS).
- 在素模型中,HNPOMOF-2NS在C-C键的氧化裂解中表现出优异的光催化活性.
结论:
- 建立了一个可行的战略,用于构建基于高核度POM集群的MOF.
- 合成的POM-MOF,特别是HNPOMOF-2NS,显示出作为绿色催化应用的高效材料的巨大潜力.
- 这项工作扩大了基于POM的材料的范围,用于先进的功能应用,包括可持续化学.
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