Abstract
It is significant to gain insights into the electronic interfacial interactions on non-reducible oxides as they can effectively improve the catalytic performance. Herein, we reported the fabrication of Au0Pdδ+ alloy (average size: 1.9 nm) co-modified with Na12[α-P2W15O56] (P2W15) nanoclusters on aluminum oxide (denoted as AuPd/P2W15-Al2O3) by deposition–precipitation and covalent immobilization strategy. The as-prepared AuPd/P2W15-Al2O3 exhibited 92 % conversion, 96 % selectivity of benzaldehyde with the reaction rate of 4.9 × 104h−1 when applied for the selective oxidation of benzyl alcohol, which was superior to AuPd/Al2O3, Au/P2W15-Al2O3 and Pd/P2W15-Al2O3 catalysts. Such excellent catalytic performance can be ascribed to the fact that: the electrons transfer from P2W15 to Au0Pdδ+ alloy resulted in the electron-rich Au0Pdδ+ alloy species, and the enhanced interfacial interactions between Au0Pdδ+ alloy and P2W15 nanoclusters facilitated activation of O2 to generate superoxide radicals •O2–. Moreover, density-functional theory (DFT) calculation confirmed that the P2W15 clusters modulated the d-band center of Au0Pdδ+ alloy and accelerated the adsorption of benzyl alcohol, O2 activation and desorption of benzaldehyde.
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