Abstract
For the oxidation reaction of isobutene to methacrolein, Mo–Bi based catalysts have attracted wide attentions in academia and industry. Current studies focus on deeply understanding reaction mechanism, pathways and catalytic active sites. However, most are only based on simple binary Mo–Bi oxides or several isolated/specific metal elements, which difficultly reflects the real reaction process on the surface of commercial catalysts. How to optimize the practical active phase structure has rarely been reported in recent years. Here we report that based on the multicomponent metal oxide Co6Fe4Mo12Bi1.5Ox active phase, Fe could be isomorphic substituted by the other elements (Cu and Ag), which is the active site for the reactant O2 activation. More importantly, the principal active site terminal oxygen Mo=O for oxidation reaction of isobutene to methacrolein could be fine-tuned via the electronic inductive effect of isomorphous-substitution elements, and then catalytic performances of the corresponding catalysts were greatly enhanced. The research provides an all-new angle of view for developing and synthetizing the ultra-high performance commercial catalysts for allylic oxidation reactions.
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Acknowledgements
We are grateful for financial support from the National Natural Science Foundation of China (grant 21706227), Key Research and Development Plan of Shandong Province (Major Scientific and Technological Innovation Project, grant 2021ZDSYS24), Science and Technology Innovation Development Plan of Yantai (grant 2020XDRH100).
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Yan, L., Yuan, Q., Tian, H. et al. Fine-tuning the active site terminal oxygen Mo=O of practical active phase via an isomorphous-substitution method for the reaction of isobutene to methacrolein. Reac Kinet Mech Cat 136, 205–216 (2023). https://doi.org/10.1007/s11144-022-02332-5
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DOI: https://doi.org/10.1007/s11144-022-02332-5