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Reactivity of Pd–MO2 encapsulated catalytic systems for CO oxidation

机译：PD – MO2封装催化系统的反应性，用于CO氧化

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摘要

In this study, we present an investigation aimed at characterizing and understanding the synergistic interactions in encapsulated catalytic structures between the metal core (i.e., Pd) and oxide shell (i.e., TiO2, ZrO2, and CeO2). Encapsulated catalysts were synthesized using a two-step procedure involving the initial colloidal synthesis of Pd nanoparticles (NPs) capped by various ligands and subsequent sol–gel encapsulation of the NPs with porous MO2 (M = Ti, Zr, Ce) shells. The encapsulated catalytic systems displayed higher activity than the Pd/MO2 supported structures due to unique physicochemical properties at the Pd–MO2 interface. Pd@ZrO2 exhibited the highest catalytic activity for CO oxidation. Results also suggested that the active sites in Pd encapsulated by an amorphous ZrO2 shell structure were significantly more active than the crystalline oxide encapsulated structures at low temperatures. Furthermore, CO DRIFTS studies showed that Pd redispersion occurred under CO oxidation reaction conditions and as a function of the oxide shell composition, being observed in Pd@TiO2 systems only, with potential formation of smaller NPs and oxide-supported Pd clusters after reaction. This investigation demonstrated that metal oxide composition and (in some cases) crystallinity play major roles in catalyst activity for encapsulated catalytic systems.
机译：在这项研究中，我们提出了一项旨在表征和理解金属芯（即PD）和氧化物壳（即TiO2，ZRO2和CEO2）之间的协同相互作用的研究。使用涉及由各种配体限制的PD纳米颗粒（NPS）的初始胶体合成的两步方法合成了封装的催化剂，以及随后用多孔MO2（M = Ti，Zr，CE）壳的NPS封装NPS的Sol-Gel封装。封装的催化系统的活性比PD – MO2接口处的独特物理化学特性，比PD/MO2支持的结构更高。 PD@ZRO2表现出用于CO氧化的最高催化活性。结果还表明，由无定形ZRO2壳结构封装的PD中的活性位点比低温下的氧化氧化物封装结构的活性明显得多。此外，CO漂移研究表明，PD重新分散发生在CO氧化反应条件下，并且是氧化物壳成分的函数，仅在PD@TiO2系统中观察到，反应后的潜在形成较小的NP和氧化物支持的PD簇。这项研究表明，金属氧化物的组成和（在某些情况下）结晶度在封装的催化系统中在催化剂活性中起主要作用。

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