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交叉形多氧金属集中的异离子的自我分类

Qi Zheng¹, Laia Vilà-Nadal¹, Zhongling Lang²

¹WestCHEM, School of Chemistry, The University of Glasgow , Glasgow G12 8QQ, United Kingdom.

Journal of the American Chemical Society

|January 24, 2018

概括

研究人员开发了一种新型的交叉形多氧金属结构,可以自行排序两个不同的异离子 (HA) 模板. 这允许在结构中精确地放置HA,从而创建具有可调节电子属性的功能分子架构.

科学领域:

无机化学
材料科学
超分子化学

背景情况:

异离子 (HA) 部分对于模拟异聚氧金属 (HPA) 架构至关重要.
由多个不同的HA部分构成的集群很少被报告,这限制了结构多样性.

研究的目的:

在单个HPA架构中研究两个不同的HA模板的自我排序.
合成和描述新型的交叉形状的HPA结构,其中包括混合HA模板.
探索内置的HA对HPA集群的电子特性的影响.

主要方法:

交叉形的多氧金属结构的自组装.
混合异模板的结合 (例如酸盐,酸盐,酸盐,酸盐).
使用单晶X射线衍射,NMR光谱和质谱学的结构特征.
使用DFT计算的计算研究.
通过微分脉冲电压测量进行电化学分析.

主要成果:

合成了一种新的十字形HPA架构,[{XYW15O54) 4{WO2) ]32/36-,能够自行排序两个不同的HA模板.
混合HA模板在结构中的确切位置被明确确定.
从溶液中优先形成和结晶混合HA模板集群.
DFT的计算表明,解决方案中的模板协调驱动了选择性自我排序.
加入的HA轻微调节了HPA团的氧化还原活性.

结论:

开发的十字形HPA显示出从溶液中选择和分类多个HA模板的显著能力.
这为构建具有明确结构和可调节电子属性的复杂HPA架构提供了途径.
这些发现为设计基于多氧金属酸盐的先进功能分子材料开辟了道路.

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