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在无溶剂条件下,单原子铂或钯掺杂的多孔二氧化铈纳米颗粒上环己烯的氢化反应。

Hydrogenation of cyclohexene over single-atom Pt or Pd incorporated porous ceria nanoparticles under solvent-free conditions.

作者信息

Atran Amal A, Hamdy Mohamed S

机构信息

Catalysis Research Group (CRG), Department of Chemistry, College of Science, King Khalid University P.O Box 9004 Abha 61413 Saudi Arabia

出版信息

RSC Adv. 2024 Apr 2;14(15):10644-10652. doi: 10.1039/d4ra01432d. eCollection 2024 Mar 26.

Abstract

In order to maximize the utilization of noble metals in catalysis, single atom of palladium (Pd) and platinum (Pt) were incorporated individually in the framework of porous ceria (CeO) by using a one-step flash combustion method. Samples with different Pd and Pt loading (0.5, 1, 2.5, and 5 wt%) were prepared and examined by using different analysis techniques such as XRD, ICP, N sorption measurements, SEM, HR-TEM, and XPS. The characterization data confirms the formation of zero-state single-atom Pt and Pd (with possible formation of Pd nanoparticles with a size less than 5 nm) incorporated onto the three-dimensional porous ceria structure. The catalytic activity of the synthesized materials was studied in the cyclohexene reduction to cyclohexane at 393 K and 3 atm of pure hydrogen (H) gas as a model reaction. The obtained results demonstrated that the conversion percentage of cyclohexene is increasing with Pd or Pt loading. The best cyclohexene conversion, 21% and 29%, was achieved over the sample that contains 5 wt% of Pt and Pd, respectively. The collected catalytic data fit the zero-order reaction model, and the rate constant of each catalyst was determined. The catalytic experiments of the most-performed catalysts were repeated five times and the obtained loss in activity was insignificant.

摘要

为了在催化过程中最大限度地利用贵金属,采用一步快速燃烧法将单个钯(Pd)原子和铂(Pt)原子分别引入多孔二氧化铈(CeO)骨架中。制备了具有不同Pd和Pt负载量(0.5、1、2.5和5 wt%)的样品,并使用XRD、ICP、N吸附测量、SEM、HR-TEM和XPS等不同分析技术进行检测。表征数据证实了零价单原子Pt和Pd的形成(可能形成尺寸小于5 nm的Pd纳米颗粒),并掺入到三维多孔二氧化铈结构中。以纯氢气(H)在393 K和3 atm下将环己烯还原为环己烷作为模型反应,研究了合成材料的催化活性。所得结果表明,环己烯的转化率随Pd或Pt负载量的增加而提高。分别在含有5 wt% Pt和Pd的样品上实现了最佳的环己烯转化率,分别为21%和29%。收集到的催化数据符合零级反应模型,并确定了每种催化剂的速率常数。对性能最佳的催化剂进行了五次催化实验,活性损失不显著。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ae8e/10985592/39f841bd6998/d4ra01432d-f1.jpg

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