Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina

Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). R...

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Veröffentlicht in:The journal of physical chemistry letters 2021-03, Vol.12 (10), p.2536-2546
Hauptverfasser: Zhao, Yutong, Wang, Lizhuo, Kochubei, Alena, Yang, Wenjie, Xu, Haimei, Luo, Yongming, Baiker, Alfons, Huang, Jun, Wang, Zichun, Jiang, Yijiao
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container_issue 10
container_start_page 2536
container_title The journal of physical chemistry letters
container_volume 12
creator Zhao, Yutong
Wang, Lizhuo
Kochubei, Alena
Yang, Wenjie
Xu, Haimei
Luo, Yongming
Baiker, Alfons
Huang, Jun
Wang, Zichun
Jiang, Yijiao
description Alumina and its mixed oxides are popular industrial supports for emerging supported metal catalysts. Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. Pt single sites supported on AlV-enriched ASA exhibit excellent chemoselectivity in the hydrogenation of CO groups, affording 2–3-fold higher yields compared to those of Pt nanoparticles supported on Al2O3 and SiO2.
doi_str_mv 10.1021/acs.jpclett.1c00139
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Pentacoordinated Al (AlV) species are identified as key surface sites for anchoring and stabilizing metal single-site catalysts; however, AlV is rare in conventional amorphous silica–alumina (ASA). Recently, we have developed AlV-enriched ASA, which was applied as a support for the synthesis of Pt single-site catalysts in this work. Each preparation stage and the interaction between Pt and surface Al species were explored by 1H and 27Al solid-state nuclear magnetic resonance spectroscopy, and the formation of the dominant Pt single sites on the surface of AlV-enriched ASA was confirmed by high-angle annular dark-field imaging scanning transmission electron microscopy and energy dispersive spectroscopy line scanning. On the surface of supports without a significant AlV population (Pt/Al2O3 and Pt/SiO2), mainly Pt nanoparticles were formed. This indicates that AlV contributes to the strong metal–support interaction to stabilize the Pt single sites on Pt/ASA, which was characterized by diffuse reflectance infrared Fourier transform spectroscopy combined with CO adsorption, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. 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title Formation and Location of Pt Single Sites Induced by Pentacoordinated Al Species on Amorphous Silica–Alumina
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