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Selective Oxidation of Isobutane to Methacrylic Acid by Metal-Substituted Ammonium Salts of Molybdovanadophosphoric Acid

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Abstract

A series of ammonium salts of molybdovanadophosphoric acid with different metal substitution and x values (abbreviated as (NH4)1.85Mx, M=Cs, Cu and Fe) were synthesized to catalyze the partial oxidation of isobutane to methacrylic acid. By XRD, TG/DTG, XRF, FT-IR, Raman spectroscopy, H2-TPR, NH3-TPD, it can be found that, compared to the un-doped (NH4)1.85H2.15PMo11VO40 catalyst, the specific surface area, amount of acid sites, and immigrating amount of V atom in Keggin unit into the secondary structure were strongly dependent on the substituted metal ions and their content. The optimum activity was obtained over (NH4)1.85Cs0.5 catalyst, which could provide a larger surface area of 37.72 m2 g−1, a higher amount of acid sites (82.47 μmol g−1), and more VO2+ species and V2O5 clusters from the immigration of V atom in Keggin structure. Furthermore, Cu-substituted catalyst accelerated the catalytic cycle of isobutane oxidation due to the higher electron-delivering efficiency, and the MAA desorption became faster and the catalysts exhibited the excellent selectivity to MAA.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 21673227), Scientific Research Project of Mudanjiang Normal University (No.1352DZ001); Innovation and Entrepreneurship Project of Mudanjiang Normal University (No.201910233025); Science and Technology Innovation Project of Mudanjiang Normal University (No.kjcx2020-024mdjnu).

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Authors and Affiliations

  1. Mudanjiang Normal University, Mudanjiang, 157011, China

    Xue Cai & Yue Ma

  2. State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Science, 457 Zhongshan Road, Dalian, 116023, Liaoning, China

    Wenling Chu & Weishen Yang

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  1. Xue Cai
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  2. Yue Ma
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  3. Wenling Chu
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  4. Weishen Yang
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Correspondence to Xue Cai or Wenling Chu.

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Cai, X., Ma, Y., Chu, W. et al. Selective Oxidation of Isobutane to Methacrylic Acid by Metal-Substituted Ammonium Salts of Molybdovanadophosphoric Acid. Catal Lett 152, 2412–2420 (2022). https://doi.org/10.1007/s10562-021-03821-3

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