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

Autor:	Tong T; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K.; Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai200237, China., Douthwaite M; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K., Chen L; Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai200237, China., Engel R; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K., Conway MB; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K., Guo W; Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai200237, China., Wu XP; Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai200237, China., Gong XQ; Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai200237, China., Wang Y; Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai200237, China., Morgan DJ; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K., Davies T; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K., Kiely CJ; Department of Materials Science and Engineering, Lehigh University, 5 East Packer Avenue, Bethlehem, Pennsylvania18015, United States., Chen L; School of Chemistry and Chemical, In-situ Centre for Physical Sciences, Frontiers Science Centre for Transformative Molecules, Shanghai Jiao Tong University, 200240Shanghai, P. R. China., Liu X; School of Chemistry and Chemical, In-situ Centre for Physical Sciences, Frontiers Science Centre for Transformative Molecules, Shanghai Jiao Tong University, 200240Shanghai, P. R. China., Hutchings GJ; Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Main Building, Park Place, CardiffCF10 3AT, U.K.
Jazyk:	angličtina
Zdroj:	ACS catalysis [ACS Catal] 2023 Jan 05; Vol. 13 (2), pp. 1207-1220. Date of Electronic Publication: 2023 Jan 05 (Print Publication: 2023).
DOI:	10.1021/acscatal.2c04347
Abstrakt:	The hydrogen-borrowing amination of alcohols is a promising route to produce amines. In this study, experimental parameters involved in the preparation of Pt/CeO 2 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 CeO 2 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 CeO 2 [100] plane, appeared to be dependent on the properties of the CeO 2 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. Competing Interests: The authors declare no competing financial interest. (© 2023 The Authors. Published by American Chemical Society.)
Databáze:	MEDLINE
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