Controlled Synthesis and Enhanced Catalytic Activity of Well-Defined Close-Contact Pd-ZnO Nanostructures.

ABSTRACT

In this study, PdZn-ordered intermetallic nanoparticles (NPs) were prepared in liquid phase by butyllithium co-reduction of their precursors at 240 °C. Through calcination and subsequent reduction with H2, the synthesized PdZn NPs were then in situ transformed into Pd-ZnO heteroaggregate nanocatalysts on alumina supports. Various characterization techniques, such as diffuse reflectance Fourier transform infrared with CO probes, transmission electron microscopy, X-ray diffraction, H2 temperature-programmed reduction, and X-ray photoelectron spectra, reveal that PdZn NPs are ordered intermetallic compounds, and in situ transformation of PdZn alloy NPs results in close-contact Pd-ZnO heteroaggregates, where the interfaces are highly active and the interaction between Pd and ZnO prevents the active particles from agglomeration. The catalytic hydrogenations of nitrophenols over Pd/Al2O3 and Pd-ZnO/Al2O3 were investigated. The results show that Pd-ZnO/Al2O3 illustrates an enhanced catalytic activity relative to Pd/Al2O3, and no obvious activity degradation was observed in the recycle catalytic experiments over such nanostructures. It is concluded that the Pd-ZnO interaction not only enhances the catalytic hydrogenation activity but also promotes the thermal and catalytic stability.