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Two sandwich-type uranyl-containing polytungstates catalyze aerobic synthesis of benzimidazoles

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Diversified synthetic strategies are extremely important for the structural diversity of uranium-containing polyoxometalates (U-POMs) and their functional expansion. Herein, two sandwich-type U-POMs were reported, which are Na5.6K6.4[(UO2)(H2O)(TeW9O33)]2·21H2O (UTeW9) and Na8.9K2.7H1.19[K0.79(UO2)2.21(PW9O34)2]·12H2O (UPW9) using in-situ strategy and lacunary precursor strategy, respectively. UTeW9 shows a typical Keggin-type open or half-sandwich configuration. UPW9 shows a typical Keggin-type sandwiched structure containing significant disorders of K(I) and uranyl ions with a triangular configuration. In addition, UTeW9 exhibits high efficiency in the catalyzed condensation of various o-arylenediamines and aldehydes for the aerobic synthesis of benzimidazoles with excellent yield.

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摘要

多样化的合成策略对含铀多金属氧簇（U-POMs）的结构多样性和功能扩展至关重要。本文分别采用原位合成策略和不稳定前驱体策略合成了两例夹心型U-POMs：Na5.6K6.4[(UO2)(H2O)(TeW9O33)]2·21H2O (UTeW9)和Na8.9K2.7H1.19[K0.79(UO22)2.21(PW99O3434)2]·12H2O (UPW9)。UTeW9是通过简单原料原位合成的，呈现出典型的Keggin型开放式或半夹心结构。UPW9由不稳定的{α-P2W12}前驱体与简单原料反应得到，呈现出典型的Keggin型夹心结构，呈三角构型的夹心中含有无序的K(I)和铀酰离子。此外，UTeW9能够高效催化各种邻芳二胺和苯甲醛的缩合反应，以优异的收率合成苯并咪唑类化合物。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (No. 22001034) and Jiangxi Provincial Natural Science Foundation (No. 20212BAB213001).

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  1. Yu-Feng Liu and Qi-Long Hu have contributed equally to this work.

Authors and Affiliations

  1. School of Chemistry and Material Science, Jiangxi Province Key Laboratory of Synthetic Chemistry, Jiangxi Key Laboratory for Mass Spectrometry and Instrumentation, East China University of Technology, Nanchang, 330013, China

    Yu-Feng Liu, Qi-Long Hu, Xue-Jiao Chen, Ke Li & Guo-** Yang

  2. School of Environmental Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China

    Pei Luo

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Liu, YF., Hu, QL., Chen, XJ. et al. Two sandwich-type uranyl-containing polytungstates catalyze aerobic synthesis of benzimidazoles. Rare Met. 43, 1316–1322 (2024). https://doi.org/10.1007/s12598-023-02532-5

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