Controlled Metal–Support Interactions in Au/CeO2–Mg(OH)2 Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate

The strong metal–support interaction (SMSI) between the three components in Au/CeO2–Mg(OH)2 can be controlled by the relative composition of CeO2 and Mg(OH)2 and by the calcination temperature for the direct...

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Autores principales:	Nagyeong Kim, Seulgi Lim, Seungdon Kwon, Yuyeol Choi, Ji-Woong Lee, Kyungsu Na
Formato:	article
Lenguaje:	EN
Publicado:	MDPI AG 2021
Materias:	oxidative esterification methacrolein methyl methacrylate Au catalyst strong metal–support interaction calcination Chemistry QD1-999
Acceso en línea:	https://doaj.org/article/4a6051178a0948f4949bd2eba72970f6
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spelling	oai:doaj.org-article:4a6051178a0948f4949bd2eba72970f62021-11-25T18:32:48ZControlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate10.3390/nano111131462079-4991https://doaj.org/article/4a6051178a0948f4949bd2eba72970f62021-11-01T00:00:00Zhttps://www.mdpi.com/2079-4991/11/11/3146https://doaj.org/toc/2079-4991The strong metal–support interaction (SMSI) between the three components in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> can be controlled by the relative composition of CeO<sub>2</sub> and Mg(OH)<sub>2</sub> and by the calcination temperature for the direct oxidative esterification of methacrolein (MACR) with methanol to methyl methacrylate (MMA). The composition ratio of CeO<sub>2</sub> and Mg(OH)<sub>2</sub> in the catalyst affects the catalytic performance dramatically. An Au/CeO<sub>2</sub> catalyst without Mg(OH)<sub>2</sub> esterified MACR to a hemiacetal species without MMA production, which confirmed that Mg(OH)<sub>2</sub> is a prerequisite for successful oxidative esterification. When Au/Mg(OH)<sub>2</sub> was used without CeO<sub>2</sub>, the direct oxidative esterification of MACR was successful and produced MMA, the desired product. However, the MMA selectivity was much lower (72.5%) than that with Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> catalysts, which have an MMA selectivity of 93.9–99.8%, depending on the relative composition of CeO<sub>2</sub> and Mg(OH)<sub>2</sub>. In addition, depending on the calcination temperature, the crystallinity of the CeO<sub>2</sub>–Mg(OH)<sub>2</sub> and the surface acidity/basicity can be remarkably changed. Consequently, the Au-nanoparticle-supported catalysts exhibited different MACR conversions and MMA selectivities. The catalytic behavior can be explained by the different metal–support interactions between the three components depending on the composition ratio of CeO<sub>2</sub> and Mg(OH)<sub>2</sub> and the calcination temperature. These differences were evidenced by X-ray diffraction, X-ray photoelectron spectroscopy, and CO<sub>2</sub> temperature-programmed desorption. The present study provides new insights into the design of SMSI-induced supported metal catalysts for the development of multifunctional heterogeneous catalysts.Nagyeong KimSeulgi LimSeungdon KwonYuyeol ChoiJi-Woong LeeKyungsu NaMDPI AGarticleoxidative esterificationmethacroleinmethyl methacrylateAu catalyststrong metal–support interactioncalcinationChemistryQD1-999ENNanomaterials, Vol 11, Iss 3146, p 3146 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	oxidative esterification methacrolein methyl methacrylate Au catalyst strong metal–support interaction calcination Chemistry QD1-999
spellingShingle	oxidative esterification methacrolein methyl methacrylate Au catalyst strong metal–support interaction calcination Chemistry QD1-999 Nagyeong Kim Seulgi Lim Seungdon Kwon Yuyeol Choi Ji-Woong Lee Kyungsu Na Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate
description	The strong metal–support interaction (SMSI) between the three components in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> can be controlled by the relative composition of CeO<sub>2</sub> and Mg(OH)<sub>2</sub> and by the calcination temperature for the direct oxidative esterification of methacrolein (MACR) with methanol to methyl methacrylate (MMA). The composition ratio of CeO<sub>2</sub> and Mg(OH)<sub>2</sub> in the catalyst affects the catalytic performance dramatically. An Au/CeO<sub>2</sub> catalyst without Mg(OH)<sub>2</sub> esterified MACR to a hemiacetal species without MMA production, which confirmed that Mg(OH)<sub>2</sub> is a prerequisite for successful oxidative esterification. When Au/Mg(OH)<sub>2</sub> was used without CeO<sub>2</sub>, the direct oxidative esterification of MACR was successful and produced MMA, the desired product. However, the MMA selectivity was much lower (72.5%) than that with Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> catalysts, which have an MMA selectivity of 93.9–99.8%, depending on the relative composition of CeO<sub>2</sub> and Mg(OH)<sub>2</sub>. In addition, depending on the calcination temperature, the crystallinity of the CeO<sub>2</sub>–Mg(OH)<sub>2</sub> and the surface acidity/basicity can be remarkably changed. Consequently, the Au-nanoparticle-supported catalysts exhibited different MACR conversions and MMA selectivities. The catalytic behavior can be explained by the different metal–support interactions between the three components depending on the composition ratio of CeO<sub>2</sub> and Mg(OH)<sub>2</sub> and the calcination temperature. These differences were evidenced by X-ray diffraction, X-ray photoelectron spectroscopy, and CO<sub>2</sub> temperature-programmed desorption. The present study provides new insights into the design of SMSI-induced supported metal catalysts for the development of multifunctional heterogeneous catalysts.
format	article
author	Nagyeong Kim Seulgi Lim Seungdon Kwon Yuyeol Choi Ji-Woong Lee Kyungsu Na
author_facet	Nagyeong Kim Seulgi Lim Seungdon Kwon Yuyeol Choi Ji-Woong Lee Kyungsu Na
author_sort	Nagyeong Kim
title	Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate
title_short	Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate
title_full	Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate
title_fullStr	Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate
title_full_unstemmed	Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate
title_sort	controlled metal–support interactions in au/ceo<sub>2</sub>–mg(oh)<sub>2</sub> catalysts activating the direct oxidative esterification of methacrolein with methanol to methyl methacrylate
publisher	MDPI AG
publishDate	2021
url	https://doaj.org/article/4a6051178a0948f4949bd2eba72970f6
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Controlled Metal–Support Interactions in Au/CeO<sub>2</sub>–Mg(OH)<sub>2</sub> Catalysts Activating the Direct Oxidative Esterification of Methacrolein with Methanol to Methyl Methacrylate

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