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      Lewis–Br⊘nsted induction acidity in SBA-15 modified with Zr and P

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          Abstract

          In this work, we present the synthesis of SBA-15 materials modified with 6 and 9 mol.% of Zr and P, respectively. Silanol SBA-15 groups were detected by Fourier transform infrared spectroscopy. X-ray diffractograms revealed that the typical hexagonal arrangement of SBA-15 was preserved after Zr and P introduction, and the structure was confirmed by transmission electron microscopy. After the Zr introduction, the morphology of SBA-15 changed from fibrous particles to a semi-spherical shape according to scanning electron microscopy, while nitrogen physisorption revealed the stability of the textural materials after the P introduction. The infrared spectra of pyridine adsorption indicated that the Zr and P incorporation into SBA-15 generated adequate Lewis and Br⊘nsted acidities to carry out methanol dehydration and direct the selectivity towards dimethyl ether, with medium-strong acid sites being responsible for obtaining up to 99% selectivity towards dimethyl ether.

          Most cited references35

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          Triblock Copolymer Syntheses of Mesoporous Silica with Periodic 50 to 300 Angstrom Pores

          D. Zhao (1998)
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            Silica-Supported, Single-Site Titanium Catalysts for Olefin Epoxidation. A Molecular Precursor Strategy for Control of Catalyst Structure

            T. Don Tilley, Jonggol Jarupatrakorn (2002)
            A molecular precursor approach involving simple grafting procedures was used to produce site-isolated titanium-supported epoxidation catalysts of high activity and selectivity. The tris(tert-butoxy)siloxy titanium complexes Ti[OSi(O(t)Bu)(3)](4) (TiSi4), ((i)PrO)Ti[OSi(O(t)Bu)(3)](3) (TiSi3), and ((t)BuO)(3)TiOSi(O(t)Bu)(3) (TiSi) react with the hydroxyl groups of amorphous Aerosil, mesoporous MCM-41, and SBA-15 via loss of HO(t)Bu and/or HOSi(O(t)Bu)(3) and introduction of titanium species onto the silica surface. Powder X-ray diffraction, nitrogen adsorption/desorption, infrared, and diffuse reflectance ultraviolet spectroscopies were used to investigate the structures and chemical natures of the surface-bound titanium species. The titanium species exist mainly in isolated, tetrahedral coordination environments. Increasing the number of siloxide ligands in the molecular precursor decreases the amount of titanium that can be introduced this way, but also enhances the catalytic activity and selectivity for the epoxidation of cyclohexene with cumene hydroperoxide as oxidant. In addition, the high surface area mesoporous silicas (MCM-41 and SBA-15) are more effective than amorphous silica as supports for these catalysts. Supporting TiSi3 on the SBA-15 affords highly active cyclohexene epoxidation catalysts (0.25-1.77 wt % Ti loading) that provide turnover frequencies (TOFs) of 500-1500 h(-1) after 1 h (TOFs are reduced by about half after calcination). These results demonstrate that oxygen-rich siloxide complexes of titanium are useful as precursors to supported epoxidation catalysts.
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              Synthesis of dimethyl ether (DME) from methanol over solid-acid catalysts

              Mingting Xu, Jack Lunsford, D.Wayne Goodman … (1997)
              Article 0 comments Cited 26 times – based on 0 reviews     Review now
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                Author and article information

                Journal
                Journal ID (publisher-id): ijmr
                Title: International Journal of Materials Research
                Publisher: Carl Hanser Verlag
                ISSN (Print): 1862-5282
                ISSN (Electronic): 2195-8556
                Publication date (Print): 16 October 2018
                Volume: 109
                Issue: 10
                Pages: 957-963
                Affiliations
                a Centro de Investigación en Petroquímica, Instituto Tecnológico de Cuidad Madero, Altamira, Tamps, México
                b Centro de Investigación en Materiales Avanzados, Chihuahua, Chih., México
                c Universidad Autónoma de San Luis Potosí, San Luis Potosí, Slp., México
                d Universidad de Colima, Facultad de Ciencias, Colima, Col., México
                Author notes
                [* ] Correspondence address, Dr. Ricardo García-Alamilla, Centro de Investigación en Petroquímica, Instituto Tecnológico de Cuidad Madero, Prolongación Bahía de Aldair, Ave. de las Bahías, 89600 Altamira, Tamps., México, Tel.: +528333574820, Fax: +528333574820, E-mail: ricardogarcia.alamilla@ 123456yahoo.com.mx
                Article
                Publisher ID: MK111697
                DOI: 10.3139/146.111697
                SO-VID: f21cfab0-6fff-429f-8781-d469222797ac
                Copyright © © 2018, Carl Hanser Verlag, München
                History
                Date received : 2 March 2018
                Date accepted : 11 May 2018
                Date: 29 August 2018
                Page count
                References: 39, Pages: 7
                Categories
                Subject: Original Contributions

                ScienceOpen disciplines: Materials technology,Materials characterization,Materials science
                Keywords: SBA-15,PO4 3– ,Methanol,Dimethyl ether,ZrO2
                Data availability:
                ScienceOpen disciplines: Materials technology, Materials characterization, Materials science
                Keywords: SBA-15, PO4 3– , Methanol, Dimethyl ether, ZrO2

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