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一个波动的多重Tm(III) - 含有开放的 Wells-Dawson 合物强化状态:合成,结构和催化应用

Guoping Yang^1,2,3, Jiawei Cao¹, Yu Xiao¹

¹Jiangxi Key Laboratory for Mass Spectrometry and Instrumentation, Jiangxi Province Key Laboratory of Functional Organic Polymers, East China University of Technology, Nanchang 330013, China.

Inorganic chemistry

|January 8, 2025

概括

合成了一种新型的富含Tm(III) 的酸,TmSiW,并证明了对乙化反应的有效催化活性. 这种化合物将多个胺离子引入到状结构中,使重要异环化合物的合成成为可能.

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:

化物酸盐是多功能多氧甲酸盐,具有多样化的应用.
将胺离子纳入这些结构可以增强它们的特性.
威尔斯-道森型[Si2W18O66]16-单元是聚氧甲酸盐化学中的一个关键组成部分.

研究的目的:

为了合成一种新的富含Tm(III) 重态,具有威尔斯-道森结构.
在有机合成中研究合成化合物的催化活性.
探索将多个胺离子纳入重态框架中的潜力.

主要方法:

使用Na10[α-SiW9O34]·18H2O,伊塔康酸和TmCl3在缓冲溶液中的水热合成.
由此产生的富含Tm(III) 重态 (TmSiW) 的结构特征.
用TmSiW进行2-aminobenzamides/2-aminobenzenesulphonamides与化物的乙化的催化评估.

主要成果:

成功合成了一种富含Tm(III) 的化物,Na{Tm3(H2O) 17[Tm2(H2O) 7(Si2W18O66) ]}·35H2O (TmSiW),具有波状1D链结构.
在TmSiW结构中识别了五个不同的Tm(III) 离子环境.
在温和的绿色条件下,tmSiW对2,3-dihydroquinazolinones和3,4-dihydro-2H-1,2,4-benzothiadiazine-1,1-dioxides的合成具有很高的催化效率.

结论:

TmSiW化合物代表了含有胺的重态的新型结构图案.
多个暴露的Tm-金属活性位点的存在使得TmSiW成为有效的异质催化剂.
这项工作为将多个胺离子纳入聚氧甲酸框架用于催化应用开辟了新的途径.

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