A self-assembly solvothermal synthesis of SiMoVn@[Cu6O(TZI)3(H2O)6]4·nH2O for the efficient selective oxidation of various alkylbenzenes
The selective oxidation of alkylbenzenes contributes greatly to the production of high-value chemicals. However, developing novel and efficient catalysts remains a great challenge. To explore new and efficient catalysts, a series of POMs of H(4+n)SiMo(12−n)VnO40 (SiMoVn, n = 1, 2 and 3) were reacted with rht-MOF-1 ([Cu6O(TZI)3(H2O)6]4·nH2O) by a one-pot self-assembly solvothermal method. As a result, three SiMoVn@rht-MOF-1 (1, n = 1; 2, n = 2 and 3, n = 3) were isolated. Single crystal analysis revealed that SiMoVn were successfully introduced in the cages of rht-MOF-1. When complex 3 was employed as a catalyst, it effectively catalyzed the selective oxidation of alkylbenzene with a conversion of 99% and selectivity of 99% under optimized reaction conditions. Recycling experiments proved that complex 3 is stable and recyclable after six cycles. In comparison with analogous catalysts, complex 3 exhibits outstanding catalytic performance. Furthermore, the kinetics and reaction mechanism were investigated and verified by EPR and XPS analysis. This approach paves a facile route to prepare POMs@MOFs for the selective oxidation of various alkylbenzenes.
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