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 in | Chemical Society reviews Vol. 44; no. 2; pp. 725 - 743 |
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| Main Authors | , , |
| Format | Journal Article |
| Language | English |
| Published |
England
21.10.2015
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| Subjects | |
| Online Access | Get full text |
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| Summary: | 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. |
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| Bibliography: | 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. ObjectType-Article-2 SourceType-Scholarly Journals-1 ObjectType-Feature-3 content type line 23 ObjectType-Review-1 |
| ISSN: | 0306-0012 1460-4744 |
| DOI: | 10.1039/c5cs00028a |