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一种含多个Tm(III)的波浪形开孔道森结构硅钨酸盐:合成、结构及催化应用

A Wavy Multiple Tm(III)-Containing Open Wells-Dawson Silicotungstate: Synthesis, Structure, and Catalytic Application.

作者信息

Yang Guoping, Cao Jiawei, Xiao Yu, Hu Qilong, Liu Haoqi, Cao Xiaohong, Li Ke, Zhang Yalin, Li Xinxiong

机构信息

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

College of Chemistry, Xinjiang University, Urumqi 830017, China.

出版信息

Inorg Chem. 2025 Jan 20;64(2):1041-1047. doi: 10.1021/acs.inorgchem.4c04468. Epub 2025 Jan 7.

DOI:10.1021/acs.inorgchem.4c04468
PMID:39772537
Abstract

A Tm(III)-rich silicotungstate Na{Tm(HO)[Tm(HO)(SiWO)]}·35HO () based on the open Wells-Dawson-type [SiWO] building unit was synthesized by the reaction of Na[α-SiWO]·18HO, itaconic acid, and TmCl in a HAc/NaAc buffer solution. Five kinds of Tm(III) ions were found in this compound and further linked the {TmSiW} subunit to form an interesting wavy 1D chain structure, which achieved the introduction of more lanthanide (Ln) ions into the [SiWO] unit for the first time. contains multiple exposed Tm-metal active sites, making it an efficient catalyst for the acetalization of 2-aminobenzamides/2-aminobenzenesulphonamides with aldehydes. A series of 2,3-dihydroquinazolinones and 3,4-dihydro-2-1,2,4-benzothiadiazine-1,1-dioxides could be obtained in excellent yields under green and mild conditions.

摘要

基于开放的韦尔斯-道森型[SiW₁₂O₄₀]构筑单元的富铥硅钨酸盐Na{Tm(OH)[Tm(OH)(SiW₁₂O₄₀)]}·35H₂O()通过在HAc/NaAc缓冲溶液中使Na[α-SiW₁₂O₄₀]·18H₂O、衣康酸和TmCl反应合成。在该化合物中发现了五种铥(III)离子,它们进一步连接{ TmSiW₁₂ }亚单元形成有趣的波浪状一维链结构,首次实现了将更多镧系(Ln)离子引入[SiW₁₂O₄₀]单元。含有多个暴露的铥金属活性位点,使其成为2-氨基苯甲酰胺/2-氨基苯磺酰胺与醛缩醛化反应的高效催化剂。在绿色温和条件下可以以优异的产率获得一系列2,3-二氢喹唑啉酮和3,4-二氢-2H-1,2,4-苯并噻二嗪-1,1-二氧化物。

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