Dataset Information

Uncovering Structure-Activity Relationships in Pt/CeO₂ Catalysts for Hydrogen-Borrowing Amination.

ABSTRACT: The hydrogen-borrowing amination of alcohols is a promising route to produce amines. In this study, experimental parameters involved in the preparation of Pt/CeO₂ catalysts were varied to assess how physicochemical properties influence their performance in such reactions. An amination reaction between cyclopentanol and cyclopentylamine was used as the model reaction for this study. The Pt precursor used in the catalyst synthesis and the properties of the CeO₂ support were both found to strongly influence catalytic performance. Aberration corrected scanning transmission electron microscopy revealed that the most active catalyst comprised linearly structured Pt species. The formation of these features, a function result of epitaxial Pt deposition along the CeO₂ [100] plane, appeared to be dependent on the properties of the CeO₂ support and the Pt precursor used. Density functional theory calculations subsequently confirmed that these sites were more effective for cyclopentanol dehydrogenation-considered to be the rate-determining step of the process-than Pt clusters and nanoparticles. This study provides insights into the desirable catalytic properties required for hydrogen-borrowing amination but has relevance to other related fields. We consider that this study will provide a foundation for further study in this atom-efficient area of chemistry.

SUBMITTER: Tong T

PROVIDER: S-EPMC9872813 | biostudies-literature | 2023 Jan

REPOSITORIES: biostudies-literature

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Uncovering Structure-Activity Relationships in Pt/CeO2 Catalysts for Hydrogen-Borrowing Amination.

Tong Tao T Douthwaite Mark M Chen Lu L Engel Rebecca R Conway Matthew B MB Guo Wanjun W Wu Xin-Ping XP Gong Xue-Qing XQ Wang Yanqin Y Morgan David J DJ Davies Thomas T Kiely Christopher J CJ Chen Liwei L Liu Xi X Hutchings Graham J GJ

ACS catalysis 20230105 2

The hydrogen-borrowing amination of alcohols is a promising route to produce amines. In this study, experimental parameters involved in the preparation of Pt/CeO2 catalysts were varied to assess how physicochemical properties influence their performance in such reactions. An amination reaction between cyclopentanol and cyclopentylamine was used as the model reaction for this study. The Pt precursor used in the catalyst synthesis and the properties of the CeO2 support were b ...[more]

PMID: 36714055

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Project description:Construction of a C-C bond via alkylation of ketones with alcohol as the alkylating source by employing hydrogen-borrowing strategy is attracting significant attention and is highly appealing due to its simplicity, cost-effectiveness, environmental benefits, and the fact that water is the only byproduct. The development of heterogeneous catalysts based on nonprecious base metals is progressing rapidly. Our newly disclosed manganese-doped cerium oxide nanocomposite (10 wt % Mn@CeO2) stands out as a cost-efficient and air-stable catalyst, synthesized through a straightforward coprecipitation method and employed for α-alkylation of ketones with primary alcohols via the hydrogen-borrowing strategy. X-ray diffraction (XRD) analysis confirms the high crystallinity of CeO2, while field emission scanning electron microscopy (FE-SEM) and high-resolution transmission electron microscopy (HR-TEM) images reveal MnO2 nanoparticles, measuring 19 nm in size, uniformly decorated on the rod-shaped CeO2 nanoparticles, which have a size of 33 nm. X-ray photoelectron spectroscopy (XPS) analysis uncovers the presence of Mn4+ species embedded on the CeO2 nanorods. Electron paramagnetic resonance (EPR) analysis further indicates that surface defects contribute to the impressive catalytic yield, which ranges from 70 to 98% for the α-alkylated ketones. Thermogravimetric analysis (TGA) demonstrates the remarkable thermal stability of the catalyst, maintaining its stability up to 800 °C. Additionally, inductively coupled plasma mass spectrometry (ICP-MS) confirms no leaching of Mn ions, emphasizing the high heterogeneity of the catalyst. Remarkably, 10 wt % Mn@CeO2 nanocomposite is recycled for six cycles with no loss of catalytic activity. This study underscores the synergistic effect between the base metal MnO2 and redox pair of CeO2, which is key to the exceptional catalytic activity in α-alkylation reactions, making 10 wt % Mn@CeO2 a highly promising catalyst for sustainable and efficient C-C bond formation.

Dataset Information

Uncovering Structure-Activity Relationships in Pt/CeO₂ Catalysts for Hydrogen-Borrowing Amination.

Publications

Uncovering Structure-Activity Relationships in Pt/CeO<sub>2</sub> Catalysts for Hydrogen-Borrowing Amination.

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