Kibis Lidiya, Zadesenets Andrey, Garkul Ilia, Korobova Arina, Kardash Tatyana, Slavinskaya Elena, Stonkus Olga, Korenev Sergey, Podyacheva Olga, Boronin Andrei
Boreskov Institute of Catalysis, Pr. Lavrentieva 5, 630090 Novosibirsk, Russia.
Nikolaev Institute of Inorganic Chemistry, Pr. Lavrentieva 3, 630090 Novosibirsk, Russia.
Materials (Basel). 2022 Oct 25;15(21):7485. doi: 10.3390/ma15217485.
The composite nanomaterials based on noble metals, reducible oxides, and nanostructured carbon are considered to be perspective catalysts for many useful reactions. In the present work, multi-walled carbon nanotubes (MWCNTs) were used for the preparation of Pd-Ce-Ox/MWCNTs and Pt-Ce-Ox/MWCNTs catalysts comprising the active components (6 wt%Pd, 6 wt%Pt, 20 wt%CeO2) as highly dispersed nanoparticles, clusters, and single atoms. The application of X-ray diffraction (XRD) and high-resolution transmission electron microscopy (HRTEM) provided analysis of the samples’ morphology and structure at the atomic level. For Pd-Ce-Ox/MWCNTs samples, the formation of PdO nanoparticles with an average crystallite size of ~8 nm was shown. Pt-Ce-Ox/MWCNTs catalysts comprised single Pt2+ ions and PtOx clusters less than 1 nm. A comparison of the catalytic properties of the samples showed higher activity of Pd-based catalysts in CO and CH4 oxidation reactions in a low-temperature range (T50 = 100 °C and T50 = 295 °C, respectively). However, oxidative pretreatment of the samples resulted in a remarkable enhancement of CO oxidation activity of Pt-Ce-Ox/MWCNTs catalyst at T < 20 °C (33% of CO conversion at T = 0 °C), while no changes were detected for the Pd-Ce-Ox/MWCNTs sample. The revealed catalytic effect was discussed in terms of the capability of the Pt-Ce-Ox/MWCNTs system to form unique PtOx clusters providing high catalytic activity in low-temperature CO oxidation.
基于贵金属、可还原氧化物和纳米结构碳的复合纳米材料被认为是许多有用反应的潜在催化剂。在本工作中,多壁碳纳米管(MWCNTs)被用于制备Pd-Ce-Ox/MWCNTs和Pt-Ce-Ox/MWCNTs催化剂,这些催化剂包含作为高度分散的纳米颗粒、团簇和单原子的活性组分(6 wt% Pd、6 wt% Pt、20 wt% CeO2)。X射线衍射(XRD)和高分辨率透射电子显微镜(HRTEM)的应用提供了对样品在原子水平上的形态和结构的分析。对于Pd-Ce-Ox/MWCNTs样品,显示出形成了平均微晶尺寸约为8 nm的PdO纳米颗粒。Pt-Ce-Ox/MWCNTs催化剂包含单个Pt2+离子和小于1 nm的PtOx团簇。样品催化性能的比较表明,在低温范围内(T50分别为100 °C和295 °C),基于Pd的催化剂在CO和CH4氧化反应中具有更高的活性。然而,样品的氧化预处理导致Pt-Ce-Ox/MWCNTs催化剂在T < 20 °C时CO氧化活性显著增强(在T = 0 °C时CO转化率为33%),而Pd-Ce-Ox/MWCNTs样品未检测到变化。根据Pt-Ce-Ox/MWCNTs体系形成独特的PtOx团簇从而在低温CO氧化中提供高催化活性的能力,对所揭示的催化效应进行了讨论。