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钯-二氧化铈/碳纳米材料复合材料作为一氧化碳和甲烷氧化的催化剂

Pd-Ceria/CNMs Composites as Catalysts for CO and CH Oxidation.

作者信息

Stonkus Olga, Kibis Lidiya, Slavinskaya Elena, Zadesenets Andrey, Garkul Ilia, Kardash Tatyana, Stadnichenko Andrey, Korenev Sergey, Podyacheva Olga, Boronin Andrei

机构信息

Boreskov Institute of Catalysis, Pr. Lavrentieva 5, 630090 Novosibirsk, Russia.

Nikolaev Institute of Inorganic Chemistry, Pr. Lavrentieva 3, 630090 Novosibirsk, Russia.

出版信息

Materials (Basel). 2023 Jun 8;16(12):4257. doi: 10.3390/ma16124257.

DOI:10.3390/ma16124257
PMID:37374441
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10302758/
Abstract

The application of composite materials as catalysts for the oxidation of CO and other toxic compounds is a promising approach for air purification. In this work, the composites comprising palladium and ceria components supported on multiwall carbon nanotubes, carbon nanofibers and Sibunit were studied in the reactions of CO and CH oxidation. The instrumental methods showed that the defective sites of carbon nanomaterials (CNMs) successfully stabilize the deposited components in a highly-dispersed state: PdO and CeO nanoparticles, subnanosized PdO and PdCeO clusters with an amorphous structure, as well as single Pd and Ce atoms, are formed. It was shown that the reactant activation process occurs on palladium species with the participation of oxygen from the ceria lattice. The presence of interblock contacts between PdO and CeO nanoparticles has an important effect on oxygen transfer, which consequently affects the catalytic activity. The morphological features of the CNMs, as well as the defect structure, have a strong influence on the particle size and mutual stabilization of the deposited PdO and CeO components. The optimal combination of highly dispersed PdO and PdCeO species, as well as PdO nanoparticles in the CNTs-based catalyst, makes it highly effective in both studied oxidation reactions.

摘要

将复合材料用作一氧化碳及其他有毒化合物氧化反应的催化剂是一种很有前景的空气净化方法。在本研究中,对负载于多壁碳纳米管、碳纳米纤维和Sibunit上的钯和二氧化铈复合材料进行了一氧化碳和甲烷氧化反应的研究。仪器分析方法表明,碳纳米材料(CNMs)的缺陷位点成功地将负载的组分稳定在高度分散的状态:形成了氧化钯和二氧化铈纳米颗粒、具有非晶态结构的亚纳米级氧化钯和钯铈氧化物团簇以及单个钯和铈原子。结果表明,反应物的活化过程发生在钯物种上,且二氧化铈晶格中的氧参与其中。氧化钯和二氧化铈纳米颗粒之间的块间接触对氧转移有重要影响,进而影响催化活性。碳纳米材料的形态特征以及缺陷结构对负载的氧化钯和二氧化铈组分的粒径和相互稳定性有很大影响。基于碳纳米管的催化剂中高度分散的氧化钯和钯铈氧化物物种以及氧化钯纳米颗粒的最佳组合,使其在上述两种氧化反应中均具有很高的效率。

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