Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio

The selective oxidation of veratryl alcohol (VA), a model compound of lignin, with oxygen molecules to produce veratraldehyde (VAld) was studied over monometallic Au, Pd, and bimetallic Au:Pd nanoparticles supported on a Ce0.62Zr0.38O2 mixed oxide for the first time. These bimetallic Au-Pd catalysts...

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Main Authors: Carol M. Olmos, Lidia E. Chinchilla, Andrea M. Cappella, Alberto Villa, Juan J. Delgado, Ana B. Hungría, Ginesa Blanco, Jose J. Calvino, Laura Prati, Xiaowei Chen
Format: Article
Language:English
Published: MDPI AG 2018-08-01
Series:Nanomaterials
Subjects:
Online Access:http://www.mdpi.com/2079-4991/8/9/669
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spelling doaj-6c84656cd3624d8f948b874dfaf6c0f52020-11-24T22:09:46ZengMDPI AGNanomaterials2079-49912018-08-018966910.3390/nano8090669nano8090669Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar RatioCarol M. Olmos0Lidia E. Chinchilla1Andrea M. Cappella2Alberto Villa3Juan J. Delgado4Ana B. Hungría5Ginesa Blanco6Jose J. Calvino7Laura Prati8Xiaowei Chen9Departamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainDepartamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainDipartimento di Chimica, Università degli Studi di Milano, I-20133 Milano, ItalyDipartimento di Chimica, Università degli Studi di Milano, I-20133 Milano, ItalyDepartamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainDepartamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainDepartamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainDepartamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainDipartimento di Chimica, Università degli Studi di Milano, I-20133 Milano, ItalyDepartamento de Ciencia de los Materiales, Ingeniería Metalúrgica y Química Inorgánica, Facultad de Ciencias, Universidad de Cádiz, Campus Río San Pedro, E-11510 Puerto Real (Cádiz), SpainThe selective oxidation of veratryl alcohol (VA), a model compound of lignin, with oxygen molecules to produce veratraldehyde (VAld) was studied over monometallic Au, Pd, and bimetallic Au:Pd nanoparticles supported on a Ce0.62Zr0.38O2 mixed oxide for the first time. These bimetallic Au-Pd catalysts with Au:Pd molar ratios from 0.4 to 4.3 were synthesized by the sol-immobilization method. Furthermore, all the catalysts were characterized by inductively coupled plasma-atomic emission spectroscopy (ICP-AES), N2 physisorption, X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy-high angle annular dark field (STEM-HAADF) imaging, energy dispersive X-ray spectroscopy (EDXS), and temperature programmed reduction (TPR) techniques. A synergistic effect between gold and palladium was observed over all the bimetallic catalysts in a wide range of studied Au:Pd ratios. Remarkably, the optimum Au:Pd ratio for this reaction was 1.4 with a turnover frequency of almost six times larger than for the monometallic gold and palladium catalysts. Selectivity to veratraldehyde was higher than 99% for the monometallic Au, Pd, and all the bimetallic Au-Pd catalysts, and stayed constant during the reaction time.http://www.mdpi.com/2079-4991/8/9/669veratryl alcohol oxidationligninbimetallic Au-Pd catalystceria-zirconiaAu:Pd molar ratio
collection DOAJ
language English
format Article
sources DOAJ
author Carol M. Olmos
Lidia E. Chinchilla
Andrea M. Cappella
Alberto Villa
Juan J. Delgado
Ana B. Hungría
Ginesa Blanco
Jose J. Calvino
Laura Prati
Xiaowei Chen
spellingShingle Carol M. Olmos
Lidia E. Chinchilla
Andrea M. Cappella
Alberto Villa
Juan J. Delgado
Ana B. Hungría
Ginesa Blanco
Jose J. Calvino
Laura Prati
Xiaowei Chen
Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio
Nanomaterials
veratryl alcohol oxidation
lignin
bimetallic Au-Pd catalyst
ceria-zirconia
Au:Pd molar ratio
author_facet Carol M. Olmos
Lidia E. Chinchilla
Andrea M. Cappella
Alberto Villa
Juan J. Delgado
Ana B. Hungría
Ginesa Blanco
Jose J. Calvino
Laura Prati
Xiaowei Chen
author_sort Carol M. Olmos
title Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio
title_short Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio
title_full Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio
title_fullStr Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio
title_full_unstemmed Selective Oxidation of Veratryl Alcohol over Au-Pd/Ce0.62Zr0.38O2 Catalysts Synthesized by Sol-Immobilization: Effect of Au:Pd Molar Ratio
title_sort selective oxidation of veratryl alcohol over au-pd/ce0.62zr0.38o2 catalysts synthesized by sol-immobilization: effect of au:pd molar ratio
publisher MDPI AG
series Nanomaterials
issn 2079-4991
publishDate 2018-08-01
description The selective oxidation of veratryl alcohol (VA), a model compound of lignin, with oxygen molecules to produce veratraldehyde (VAld) was studied over monometallic Au, Pd, and bimetallic Au:Pd nanoparticles supported on a Ce0.62Zr0.38O2 mixed oxide for the first time. These bimetallic Au-Pd catalysts with Au:Pd molar ratios from 0.4 to 4.3 were synthesized by the sol-immobilization method. Furthermore, all the catalysts were characterized by inductively coupled plasma-atomic emission spectroscopy (ICP-AES), N2 physisorption, X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy-high angle annular dark field (STEM-HAADF) imaging, energy dispersive X-ray spectroscopy (EDXS), and temperature programmed reduction (TPR) techniques. A synergistic effect between gold and palladium was observed over all the bimetallic catalysts in a wide range of studied Au:Pd ratios. Remarkably, the optimum Au:Pd ratio for this reaction was 1.4 with a turnover frequency of almost six times larger than for the monometallic gold and palladium catalysts. Selectivity to veratraldehyde was higher than 99% for the monometallic Au, Pd, and all the bimetallic Au-Pd catalysts, and stayed constant during the reaction time.
topic veratryl alcohol oxidation
lignin
bimetallic Au-Pd catalyst
ceria-zirconia
Au:Pd molar ratio
url http://www.mdpi.com/2079-4991/8/9/669
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