Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate

Bimetallic zeolite Beta in bead format and containing Al sites with Brønsted acid behavior and Sn, Zr or Hf sites with Lewis acid character, were prepared using a two-step synthetic route. First, zeolite Beta in the format of macroscopic beads (400 to 840 μm) with hierarchical porosity (micropores a...

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Autores principales:	Zahra Asgar Pour, Dina G. Boer, Shun Fang, Zhenchen Tang, Paolo P. Pescarmona
Formato:	article
Lenguaje:	EN
Publicado:	MDPI AG 2021
Materias:	methyl lactate Sn-Al-Beta zeolite hierarchical zeolites Lewis acid zeolites shaped catalysts glycerol conversion Chemical technology TP1-1185 Chemistry QD1-999
Acceso en línea:	https://doaj.org/article/3ecbfe649fc44c37b3374343364a3d84
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spelling	oai:doaj.org-article:3ecbfe649fc44c37b3374343364a3d842021-11-25T17:06:09ZBimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate10.3390/catal111113462073-4344https://doaj.org/article/3ecbfe649fc44c37b3374343364a3d842021-11-01T00:00:00Zhttps://www.mdpi.com/2073-4344/11/11/1346https://doaj.org/toc/2073-4344Bimetallic zeolite Beta in bead format and containing Al sites with Brønsted acid behavior and Sn, Zr or Hf sites with Lewis acid character, were prepared using a two-step synthetic route. First, zeolite Beta in the format of macroscopic beads (400 to 840 μm) with hierarchical porosity (micropores accessed through meso- and macropores in the range of 30 to 150 nm) were synthesized by hydrothermal crystallization in the presence of anion-exchange resin beads as hard template and further converted into their H-form. Next, the zeolite beads were partially dealuminated using different concentrations of HNO<sub>3</sub> (i.e., 1.8 or 7.2 M), followed by grafting with one of the above-mentioned metals (Sn, Zr or Hf) to introduce Lewis acid sites. These bimetallic zeolites were tested as heterogeneous catalysts in the conversion of dihydroxyacetone (DHA) to methyl lactate (ML). The Sn-containing zeolite Beta beads treated by 1.8 M HNO<sub>3</sub> and grafted with 27 mmol of SnCl<sub>4</sub> (Sn-deAl-1.8-Beta-B) demonstrated the best catalytic activity among the prepared bimetallic zeolite beads, with 99% selectivity and 90% yield of ML after 6 h at 90 °C. This catalyst was also tested in combination with Au-Pd nanoparticles supported on functionalized carbon nanotubes (CNTs) as multifunctional catalytic system for the conversion of glycerol to ML, achieving 29% conversion of glycerol and 67% selectivity towards ML after 4.5 h at 140 °C under 30 bar air. The catalytic results were rationalized by means of a thorough characterization of the zeolitic beads with a combination of techniques (XRD, N<sub>2</sub>-physisorption, SEM, XRF, TEM, UV-vis spectroscopy and pyridine-FT-IR).Zahra Asgar PourDina G. BoerShun FangZhenchen TangPaolo P. PescarmonaMDPI AGarticlemethyl lactateSn-Al-Beta zeolitehierarchical zeolitesLewis acid zeolitesshaped catalystsglycerol conversionChemical technologyTP1-1185ChemistryQD1-999ENCatalysts, Vol 11, Iss 1346, p 1346 (2021)
institution	DOAJ
collection	DOAJ
language	EN
topic	methyl lactate Sn-Al-Beta zeolite hierarchical zeolites Lewis acid zeolites shaped catalysts glycerol conversion Chemical technology TP1-1185 Chemistry QD1-999
spellingShingle	methyl lactate Sn-Al-Beta zeolite hierarchical zeolites Lewis acid zeolites shaped catalysts glycerol conversion Chemical technology TP1-1185 Chemistry QD1-999 Zahra Asgar Pour Dina G. Boer Shun Fang Zhenchen Tang Paolo P. Pescarmona Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate
description	Bimetallic zeolite Beta in bead format and containing Al sites with Brønsted acid behavior and Sn, Zr or Hf sites with Lewis acid character, were prepared using a two-step synthetic route. First, zeolite Beta in the format of macroscopic beads (400 to 840 μm) with hierarchical porosity (micropores accessed through meso- and macropores in the range of 30 to 150 nm) were synthesized by hydrothermal crystallization in the presence of anion-exchange resin beads as hard template and further converted into their H-form. Next, the zeolite beads were partially dealuminated using different concentrations of HNO<sub>3</sub> (i.e., 1.8 or 7.2 M), followed by grafting with one of the above-mentioned metals (Sn, Zr or Hf) to introduce Lewis acid sites. These bimetallic zeolites were tested as heterogeneous catalysts in the conversion of dihydroxyacetone (DHA) to methyl lactate (ML). The Sn-containing zeolite Beta beads treated by 1.8 M HNO<sub>3</sub> and grafted with 27 mmol of SnCl<sub>4</sub> (Sn-deAl-1.8-Beta-B) demonstrated the best catalytic activity among the prepared bimetallic zeolite beads, with 99% selectivity and 90% yield of ML after 6 h at 90 °C. This catalyst was also tested in combination with Au-Pd nanoparticles supported on functionalized carbon nanotubes (CNTs) as multifunctional catalytic system for the conversion of glycerol to ML, achieving 29% conversion of glycerol and 67% selectivity towards ML after 4.5 h at 140 °C under 30 bar air. The catalytic results were rationalized by means of a thorough characterization of the zeolitic beads with a combination of techniques (XRD, N<sub>2</sub>-physisorption, SEM, XRF, TEM, UV-vis spectroscopy and pyridine-FT-IR).
format	article
author	Zahra Asgar Pour Dina G. Boer Shun Fang Zhenchen Tang Paolo P. Pescarmona
author_facet	Zahra Asgar Pour Dina G. Boer Shun Fang Zhenchen Tang Paolo P. Pescarmona
author_sort	Zahra Asgar Pour
title	Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate
title_short	Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate
title_full	Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate
title_fullStr	Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate
title_full_unstemmed	Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate
title_sort	bimetallic zeolite beta beads with hierarchical porosity as brønsted-lewis solid acid catalysts for the synthesis of methyl lactate
publisher	MDPI AG
publishDate	2021
url	https://doaj.org/article/3ecbfe649fc44c37b3374343364a3d84
work_keys_str_mv	AT zahraasgarpour bimetalliczeolitebetabeadswithhierarchicalporosityasbrønstedlewissolidacidcatalystsforthesynthesisofmethyllactate AT dinagboer bimetalliczeolitebetabeadswithhierarchicalporosityasbrønstedlewissolidacidcatalystsforthesynthesisofmethyllactate AT shunfang bimetalliczeolitebetabeadswithhierarchicalporosityasbrønstedlewissolidacidcatalystsforthesynthesisofmethyllactate AT zhenchentang bimetalliczeolitebetabeadswithhierarchicalporosityasbrønstedlewissolidacidcatalystsforthesynthesisofmethyllactate AT paoloppescarmona bimetalliczeolitebetabeadswithhierarchicalporosityasbrønstedlewissolidacidcatalystsforthesynthesisofmethyllactate
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Bimetallic Zeolite Beta Beads with Hierarchical Porosity as Brønsted-Lewis Solid Acid Catalysts for the Synthesis of Methyl Lactate

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