Design of Lewis-acid centres in zeolitic matrices for the conversion of renewables

The catalytic conversion of renewable feedstocks into chemicals is pursued as a means to sustainably fulfil future societal needs. Due to the oxygen-rich nature of bio-derived substrates, isomerisation, transfer-hydrogenation and retro-aldol reactions have emerged as relevant transformations to prod...

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Published inChemical Society reviews Vol. 44; no. 2; pp. 725 - 743
Main Authors Dapsens, Pierre Y, Mondelli, Cecilia, Pérez-Ramírez, Javier
Format Journal Article
LanguageEnglish
Published England 21.10.2015
Subjects
Conservation of Natural Resources
Lewis Acids - chemical synthesis
Lewis Acids - chemistry
Particle Size
Porosity
Surface Properties
Zeolites - chemistry
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Abstract The catalytic conversion of renewable feedstocks into chemicals is pursued as a means to sustainably fulfil future societal needs. Due to the oxygen-rich nature of bio-derived substrates, isomerisation, transfer-hydrogenation and retro-aldol reactions have emerged as relevant transformations to produce commodity chemicals and polymer building blocks. In this context, porous materials containing Lewis-acid metals ( e.g. , Al, Ga, Sn, Ti, Zr) play an important role. Among these, tin-containing zeolites have demonstrated superior catalytic properties which have mainly been attributed to their hydrophobicity and crystallinity. This review evaluates the versatility and the scalability of bottom-up and top-down approaches to introduce Lewis-acid functionalities in zeolitic matrices. A precise characterisation is shown to be crucial to determine the structure, acidity and environment of the sites introduced. In this regard, we highlight the limitations of conventional techniques and the advantages of analytical and modelling tools recently applied to gain an improved understanding of these solids. Thereafter, property-performance relations and important aspects for the industrial amenability of new synthetic routes are exemplified through case studies. Finally, we put forward the need for gathering deeper knowledge of the site location, surface properties and stability to aid the design of next-generation Lewis-acid catalysts. We review preparative approaches to introduce Lewis-acid centres in zeolites, underlining the structure-performance relationship and highlighting directions to design improved materials of practical relevance.
AbstractList The catalytic conversion of renewable feedstocks into chemicals is pursued as a means to sustainably fulfil future societal needs. Due to the oxygen-rich nature of bio-derived substrates, isomerisation, transfer-hydrogenation and retro-aldol reactions have emerged as relevant transformations to produce commodity chemicals and polymer building blocks. In this context, porous materials containing Lewis-acid metals (e.g., Al, Ga, Sn, Ti, Zr) play an important role. Among these, tin-containing zeolites have demonstrated superior catalytic properties which have mainly been attributed to their hydrophobicity and crystallinity. This review evaluates the versatility and the scalability of bottom-up and top-down approaches to introduce Lewis-acid functionalities in zeolitic matrices. A precise characterisation is shown to be crucial to determine the structure, acidity and environment of the sites introduced. In this regard, we highlight the limitations of conventional techniques and the advantages of analytical and modelling tools recently applied to gain an improved understanding of these solids. Thereafter, property-performance relations and important aspects for the industrial amenability of new synthetic routes are exemplified through case studies. Finally, we put forward the need for gathering deeper knowledge of the site location, surface properties and stability to aid the design of next-generation Lewis-acid catalysts.
The catalytic conversion of renewable feedstocks into chemicals is pursued as a means to sustainably fulfil future societal needs. Due to the oxygen-rich nature of bio-derived substrates, isomerisation, transfer-hydrogenation and retro-aldol reactions have emerged as relevant transformations to produce commodity chemicals and polymer building blocks. In this context, porous materials containing Lewis-acid metals ( e.g. , Al, Ga, Sn, Ti, Zr) play an important role. Among these, tin-containing zeolites have demonstrated superior catalytic properties which have mainly been attributed to their hydrophobicity and crystallinity. This review evaluates the versatility and the scalability of bottom-up and top-down approaches to introduce Lewis-acid functionalities in zeolitic matrices. A precise characterisation is shown to be crucial to determine the structure, acidity and environment of the sites introduced. In this regard, we highlight the limitations of conventional techniques and the advantages of analytical and modelling tools recently applied to gain an improved understanding of these solids. Thereafter, property-performance relations and important aspects for the industrial amenability of new synthetic routes are exemplified through case studies. Finally, we put forward the need for gathering deeper knowledge of the site location, surface properties and stability to aid the design of next-generation Lewis-acid catalysts. We review preparative approaches to introduce Lewis-acid centres in zeolites, underlining the structure-performance relationship and highlighting directions to design improved materials of practical relevance.
The catalytic conversion of renewable feedstocks into chemicals is pursued as a means to sustainably fulfil future societal needs. Due to the oxygen-rich nature of bio-derived substrates, isomerisation, transfer-hydrogenation and retro-aldol reactions have emerged as relevant transformations to produce commodity chemicals and polymer building blocks. In this context, porous materials containing Lewis-acid metals ( e.g. , Al, Ga, Sn, Ti, Zr) play an important role. Among these, tin-containing zeolites have demonstrated superior catalytic properties which have mainly been attributed to their hydrophobicity and crystallinity. This review evaluates the versatility and the scalability of bottom-up and top-down approaches to introduce Lewis-acid functionalities in zeolitic matrices. A precise characterisation is shown to be crucial to determine the structure, acidity and environment of the sites introduced. In this regard, we highlight the limitations of conventional techniques and the advantages of analytical and modelling tools recently applied to gain an improved understanding of these solids. Thereafter, property–performance relations and important aspects for the industrial amenability of new synthetic routes are exemplified through case studies. Finally, we put forward the need for gathering deeper knowledge of the site location, surface properties and stability to aid the design of next-generation Lewis-acid catalysts.
Author Pérez-Ramírez, Javier
Dapsens, Pierre Y
Mondelli, Cecilia
AuthorAffiliation ETH Zurich
Institute for Chemical and Bioengineering
Department of Chemistry and Applied Biosciences
AuthorAffiliation_xml – name: Department of Chemistry and Applied Biosciences
– name: Institute for Chemical and Bioengineering
– name: ETH Zurich
Author_xml – sequence: 1
  givenname: Pierre Y
  surname: Dapsens
  fullname: Dapsens, Pierre Y
– sequence: 2
  givenname: Cecilia
  surname: Mondelli
  fullname: Mondelli, Cecilia
– sequence: 3
  givenname: Javier
  surname: Pérez-Ramírez
  fullname: Pérez-Ramírez, Javier
BackLink https://www.ncbi.nlm.nih.gov/pubmed/25917850$$D View this record in MEDLINE/PubMed
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IngestDate Thu Oct 24 23:14:40 EDT 2024
Thu Sep 26 16:57:32 EDT 2024
Sat Sep 28 08:09:35 EDT 2024
Thu May 19 04:24:44 EDT 2016
Wed Jun 05 04:40:39 EDT 2019
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Notes Cecilia Mondelli (Como, Italy, 1979) studied Chemistry at the University of Insubria, Italy. She completed her PhD degree performing in situ infrared studies of heterogeneously catalysed reactions under the supervision of Dr R. Psaro at the University of Milan, Italy, in 2007. She then moved to ETH Zurich to continue activities in the same research field as a postdoctoral fellow in the group of Prof. A. Baiker. In 2010, she joined the group of Prof. J. Pérez-Ramírez at the same institution where she has been working as a scientist since 2011. Currently, her research mainly focuses on the conversion of biomass to chemicals over tailored catalytic systems.
2
to valuable chemicals.
Javier Pérez-Ramírez (Benidorm, Spain, 1974) studied Chemical Engineering at the University of Alicante, Spain and earned his PhD degree at TUDelft, Netherlands in 2002. Since 2010, he has been a full professor of Catalysis Engineering at the Institute for Chemical and Bioengineering of ETH Zurich. He is engaged in the discovery and the understanding of heterogeneous catalysts, multifunctional materials, and reactor engineering concepts devoted to sustainable technologies. Current topics of interest include hierarchically structured zeolites, fundamentals of the catalyst scale up, alkane functionalization, and the conversion of renewables and CO
Pierre Y. Dapsens (Namur, Belgium, 1984) completed his Master's Degree in Chemistry at the University of Namur in 2010. His Master thesis in the group of Prof. B.-L. Su focused on the development of highly ordered mesoporous hafnium silicates using a single molecular precursor. He then moved to Iowa State University to the group of Prof. B. H. Shanks to study the formation mechanism of macropores in the spontaneous self-assembly process of hierarchical metal oxides. In 2011, he joined the group of Prof. J. Pérez-Ramírez as a doctoral student. His research centres on the chemocatalytic conversion of biomass and in the development of new synthetic routes to prepare Lewis-acid zeolites.
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Snippet The catalytic conversion of renewable feedstocks into chemicals is pursued as a means to sustainably fulfil future societal needs. Due to the oxygen-rich...
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SubjectTerms Conservation of Natural Resources
Lewis Acids - chemical synthesis
Lewis Acids - chemistry
Particle Size
Porosity
Surface Properties
Zeolites - chemistry
Title Design of Lewis-acid centres in zeolitic matrices for the conversion of renewables
URI https://www.ncbi.nlm.nih.gov/pubmed/25917850
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