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Four unprecedented V14 clusters as highly efficient heterogeneous catalyst for CO2 fixation with epoxides and oxidation of sulfides

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Abstract

Chemical fixation of carbon dioxide (CO2) is an energy-saving method for alleviating the greenhouse gas emissions, whereas it persists a challenge posed by the demand for efficient catalysts. Herein, four unprecedented examples of tetradecanuclear vanadium clusters, namely, [(C2H8N2)6(CH3O)8(CH3OH)2VIV10VV4O26] (V14−1), [(C3H10N2)6(CH3O)8(CH3OH)2VIV10VV4O26](V14−2), [(C6H14N2)6(CH3O)8(CH3OH)2VIV10VV4O26]·5H2O (V14−3) and [(C4H12N2O)4(C4H11N2O)2(CH3O)2VIV10VV4O28]·6H2O (V14−4), have been triumphantly designed and constructed under solvothermal conditions. Among them, compounds V14−1–4 are the first cases of tetradecanuclear vanadium clusters without the introduction of inorganic acid radical ions. Two main units [VIV10VV4O26]8+ and [VIV10VV4O28]4+ represent brand-new configurations of tetradecanuclear vanadium clusters. Given the fact that the presence of VIV/VV can potentially facilitate electron transfer and consequently expedite catalytic reactions, we explored the catalytic activities of these compounds. Remarkably, V14−1 was further used as a heterogeneous catalyst in the CO2 fixation into cyclic carbonates under milder conditions (60 °C, 0.5 MPa) and exhibited higher catalytic activity. Also, the experimental results indicated that V14−1 could efficiently catalyze the sulfoxidation, which could fully convert most sulfides within 40 min at room temperature. Moreover, as a stable heterogeneous catalyst employed in CO2 fixation with epoxides and oxidation of sulfides, V14−1 could be consecutively used multiple cycles without losing its catalytic activity.

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Acknowledgements

This work was supported by the Natural Science Foundation of Jiangsu (BK20191359), the National Natural Science Foundation of China (92161109), the Postgraduate Research & Practice Innovation Program of Jiangsu Province (KYCX22_1343) and the Social Science Foundation of Jiangsu (19TQB002). We gratefully acknowledge the support from Prof. Qiong Zhang (Anhui University) in theoretical calculations.

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Authors and Affiliations

  1. State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing, 210009, China

    Ji-Lei Wang, Jia-Peng Cao, Yin-Hua Zhu, Qin Wang, Ning-Fang Li, Xin-Rong Fan, Hua Mei & Yan Xu

  2. State Key Laboratory of Coordination Chemistry, Coordination Chemistry Institute, Nanjing University, Nanjing, 210093, China

    Yan Xu

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  1. Ji-Lei Wang
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  2. Jia-Peng Cao
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  7. Hua Mei
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Correspondence to Hua Mei or Yan Xu.

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Conflict of interest The authors declare no conflict of interest.

Supporting information The supporting information is available online at https://chem.scichina.com and https://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Wang, JL., Cao, JP., Zhu, YH. et al. Four unprecedented V14 clusters as highly efficient heterogeneous catalyst for CO2 fixation with epoxides and oxidation of sulfides. Sci. China Chem. 66, 107–116 (2023). https://doi.org/10.1007/s11426-022-1424-9

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