Han Yong, a researcher at the State Key Laboratory of Coal Conversion in the Institute of Coal Chemistry of the Chinese Academy of Sciences, led the research team and used atomic layer deposition (ALD) to design and fabricate a metal-oxide system interface based on the tube casing structure. The tandem catalyst was used as an example, and Ni/Al2O3 and Pt/TiO2 catalysts were used as an example. The hydrogenation of hydrazine hydrazine and the hydrogenation of nitrobenzene were used as the probe series reaction, confirming the design concept of this multi-interface catalyst. Advantage. Its excellent performance can be attributed to the synergy between the two interfaces and the limited-domain nano-space favors the rapid transfer of reactive intermediates (active hydrogen). Relevant work was recently published in Angew. Chem. Int. Ed. DOI: 10.1002/ange.201600799 and was reviewed by the reviewers as a VIP (Top 5%) article.
Most chemical processes require multi-step reactions to obtain the target product, the atomic utilization of the reaction raw materials is low, and the operation steps of the reaction and purification unit are numerous, resulting in higher costs and energy consumption. The multi-step reaction can achieve one-step high-efficiency conversion, which will significantly increase the utilization of raw materials, simplify the reaction and purification process, and reduce energy consumption. Supported nanometal catalysts are the most widely used heterogeneous catalysts. The catalytic properties of metal nanoparticles can be regulated by changing their composition, morphology, size, crystal plane structure and metal-oxide interface structure. Integrating different metal-oxide interfaces into one nanoreactor can result in novel series catalysts. However, it is difficult to achieve the fine control of composition and microstructure of multi-interface catalysts by traditional catalyst preparation methods.
ALD is an advanced thin film deposition technology. By using the technical features and advantages of ALD, a new type of highly efficient nanocatalyst can be designed and the surface interface structure of the catalyst can be precisely controlled. The research team used ALD technology to form a Ni/Al2O3 interface by successively depositing Al2O3 layers and NiO nanoparticles on the template surface using carbon nano spirals or carbon nanotubes as templates; then, a polyimide film was deposited as a sacrificial layer; Pt nanoparticles and TiO2 layer were successively deposited on the surface to obtain the Pt/TiO2 interface; after calcination and reduction treatment, a dual-interface catalyst (Al/Ni-Pt/Ti) with tube interface with both Ni/Al2O3 and Pt/TiO2 interfaces was obtained. The spacing between the interfaces can be regulated by changing the film thickness of the polyimide sacrificial layer (Figure 1, Figure 2). The activity of this catalyst in the series reaction of hydrogenation of hydrazine hydride and hydrogenation of nitrobenzene is significantly higher than that of the single-interface catalyst (Al/Ni-Ti and Al-Pt/Ti) and the single-interface catalyst physical mixture (Al/Ni-Ti + Al -Pt/Ti or Ni/Al + Pt/Ti) properties. The systematic characterization and control experiments show that the active hydrogen can be rapidly transferred between the two interfaces through the nano-confined space. The active hydrogen decomposed from the Ni/Al2O3 interface of hydrazine hydride can be transferred to the Pt/TiO2 interface and participate in the reaction without hydrogen desorption. Hydrogenation of benzylbenzene skips the hydrogen activation cascade pathway and promotes efficient in-line reaction (Figure 3).
The method is universal and can be used to synthesize multi-interface catalysts in other systems for the realization of novel high-efficiency series catalysis processes. It provides an important scientific reference for the design of high-efficiency nanocatalysts in the future.
In addition, the team's previous work also used ALD to synthesize multiple-constrained nanocatalysts and ultra-thin modified multiple-restricted catalysts, which significantly improved catalyst performance by fine-tuning the metal-oxide interface structure and sites. Related work was published in Angew. Chem. Int. Ed. 2015, 54, 9006-9010; Chem. Eur. J., 2016, DOI: 10.1002/chem.201601039 (Cover paper).
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