Hongqiang Li , Wan-Lei Zhao , Wei Chen , Ruoxuan Zheng , Sai An , Yu-Fei Song
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引用次数: 0
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.
期刊介绍:
Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline.
Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.