{"title":"Catalysts for the non-oxidative dehydrogenation of ethanol supported by WO3-based micro-mesoporous composites","authors":"S. Said, M. Riad","doi":"10.1016/j.jpcs.2025.112789","DOIUrl":null,"url":null,"abstract":"<div><div>Much work has been done on synthesizing materials that enhance the conversion and selectivity of catalysts in industries by combining the stability and acidity benefits of zeolites with those of mesoporous materials. As an alternative to conventional copper oxide-supported catalysts, this study describes the synthesis of novel WO<sub>3</sub>-supported micro-mesoporous composites made of AlSBA-15 (Si/Al = 5) and various zeolites types, either HZSM-5 (MFI) or HY (FAU), using a simple deposition technique. These composites are effective catalysts for the non-oxidative dehydrogenation of ethanol to acetaldehyde. Several spectroscopic techniques were used to determine the impact of employing different zeolite types on the physicochemical characteristics of the produced micro-mesoporous composites. Additionally, their catalytic performances were evaluated when compared to the non-oxidative dehydrogenation of ethanol, utilizing a flow system to produce more valuable products. Several spectroscopic methods demonstrated that this simple synthesis approach successfully included the used zeolite-type seeds into the matrix bulk of the AlSBA-15(5). In contrast to their constituent components, the synthesized WO<sub>3</sub>-supported micro-mesoporous catalysts exhibit finer dispersion, basicity, a newly formed peak in the XPS O1S spectra due to W–O–W bridging oxygens, and comparatively higher amounts of isolated tetrahedrally monomeric WO<sub>4</sub><sup>2−</sup> (W<img>O) species to oligomeric ones. The type of zeolite used in the micro-mesoporous composite's synthesis has a significant impact on composites' catalytic performance. With a selectivity of around 96 %, the WO<sub>3</sub>-supported micro-mesoporous composite catalyst using HZSM-5 as the zeolite component demonstrates exceptional selectivity for the non-oxidative dehydrogenation of ethanol only to acetaldehyde. On the other hand, with an ethanol conversion of about 85 % at 450 °C, the WO<sub>3</sub>-supported micro-mesoporous composite catalyst used in the HY zeolite type exhibits the highest catalytic activity in terms of conversion. The catalyst's basicity, the presence of W–O–W bridges, and the comparatively higher amounts of isolated tetrahedral monomeric to oligomeric WO<sub>4</sub><sup>2−</sup> species all had a significant impact on the ethanol conversion and product selectivities during the non-oxidative dehydrogenation of ethanol.</div></div>","PeriodicalId":16811,"journal":{"name":"Journal of Physics and Chemistry of Solids","volume":"205 ","pages":"Article 112789"},"PeriodicalIF":4.3000,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Physics and Chemistry of Solids","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0022369725002410","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Much work has been done on synthesizing materials that enhance the conversion and selectivity of catalysts in industries by combining the stability and acidity benefits of zeolites with those of mesoporous materials. As an alternative to conventional copper oxide-supported catalysts, this study describes the synthesis of novel WO3-supported micro-mesoporous composites made of AlSBA-15 (Si/Al = 5) and various zeolites types, either HZSM-5 (MFI) or HY (FAU), using a simple deposition technique. These composites are effective catalysts for the non-oxidative dehydrogenation of ethanol to acetaldehyde. Several spectroscopic techniques were used to determine the impact of employing different zeolite types on the physicochemical characteristics of the produced micro-mesoporous composites. Additionally, their catalytic performances were evaluated when compared to the non-oxidative dehydrogenation of ethanol, utilizing a flow system to produce more valuable products. Several spectroscopic methods demonstrated that this simple synthesis approach successfully included the used zeolite-type seeds into the matrix bulk of the AlSBA-15(5). In contrast to their constituent components, the synthesized WO3-supported micro-mesoporous catalysts exhibit finer dispersion, basicity, a newly formed peak in the XPS O1S spectra due to W–O–W bridging oxygens, and comparatively higher amounts of isolated tetrahedrally monomeric WO42− (WO) species to oligomeric ones. The type of zeolite used in the micro-mesoporous composite's synthesis has a significant impact on composites' catalytic performance. With a selectivity of around 96 %, the WO3-supported micro-mesoporous composite catalyst using HZSM-5 as the zeolite component demonstrates exceptional selectivity for the non-oxidative dehydrogenation of ethanol only to acetaldehyde. On the other hand, with an ethanol conversion of about 85 % at 450 °C, the WO3-supported micro-mesoporous composite catalyst used in the HY zeolite type exhibits the highest catalytic activity in terms of conversion. The catalyst's basicity, the presence of W–O–W bridges, and the comparatively higher amounts of isolated tetrahedral monomeric to oligomeric WO42− species all had a significant impact on the ethanol conversion and product selectivities during the non-oxidative dehydrogenation of ethanol.
期刊介绍:
The Journal of Physics and Chemistry of Solids is a well-established international medium for publication of archival research in condensed matter and materials sciences. Areas of interest broadly include experimental and theoretical research on electronic, magnetic, spectroscopic and structural properties as well as the statistical mechanics and thermodynamics of materials. The focus is on gaining physical and chemical insight into the properties and potential applications of condensed matter systems.
Within the broad scope of the journal, beyond regular contributions, the editors have identified submissions in the following areas of physics and chemistry of solids to be of special current interest to the journal:
Low-dimensional systems
Exotic states of quantum electron matter including topological phases
Energy conversion and storage
Interfaces, nanoparticles and catalysts.