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| Naji, M. |
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| Motta, Antonella |
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| Aletan, Dirar |
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| Mohamed, Tarek |
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| Ertürk, Emre |
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| Taccardi, Nicola |
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| Kononenko, Denys |
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| Petrov, R. H. | Madrid |
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| Alshaaer, Mazen | Brussels |
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| Bih, L. |
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| Casati, R. |
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| Muller, Hermance |
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| Kočí, Jan | Prague |
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| Šuljagić, Marija |
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| Kalteremidou, Kalliopi-Artemi | Brussels |
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| Azam, Siraj |
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| Ospanova, Alyiya |
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| Blanpain, Bart |
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| Ali, M. A. |
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| Popa, V. |
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| Rančić, M. |
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| Ollier, Nadège |
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| Azevedo, Nuno Monteiro |
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| Landes, Michael |
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| Rignanese, Gian-Marco |
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Raja, Robert
University of Southampton
in Cooperation with on an Cooperation-Score of 37%
Topics
Publications (9/9 displayed)
- 2023Using small angle neutron scattering to explore porosity, connectivity and accessibility, towards optimised hierarchical solid acid catalystscitations
- 2022New insights in establishing the structure-property relations of novel plasmonic nanostructures for clean energy applicationscitations
- 2021Rational design and application of covalent organic frameworks for solar fuel productioncitations
- 2020Combining photocatalysis and optical fibre technology towards improved microreactor design for hydrogen generation with metallic nanoparticlescitations
- 2020Incorporating metal organic frameworks within microstructured optical fibers toward scalable photoreactorscitations
- 2017Heterogeneous zeotype catalysts for the direct utilisation of CO2
- 2017The molecular design of active sites in nanoporous materials for sustainable catalysiscitations
- 2013Investigating site-specific interactions and probing their role in modifying the acid-strength in framework architecturescitations
- 2009Designed nanoporous solids for the green production of vitamins, fine chemicals and renewable nylonscitations
Places of action
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document
Heterogeneous zeotype catalysts for the direct utilisation of CO2
Abstract
Due to the increasing levels of carbon dioxide (CO<sub>2</sub>) in the atmosphere, there is a growing demand for carbon utilisation technologies.Mono- and polycarbonate materials, synthesised via the catalytic conversion of CO<sub>2</sub> within the pores of high surface area materials, are providing opportunities for the sustainable development of carbon capture and utilisation (CCU) technologies.1 At this conference, we will present our most recent design strategies which utilise single-site organo-catalysts inside the pores of a zeotype framework for the formation of cyclic carbonates from CO<sub>2</sub> and epoxides. (Figure 1).<br/><br/>Due to the coordinatively unsaturated chromium nodes and large surface area, metal organic framework (MOF) MIL-101(Cr) has been identified as a suitable host for anchoring imidazole-based organo-catalysts.2A series of substituted imidazoles were synthesized and coordinated to the MOF at the chromium sites via the unsubstituted N-atom. The series was chosen to provide increasing steric demand in the imidazole side group.Characterisation of the catalyst was conducted by electron paramagnetic resonance (EPR) spectroscopy to probe the Cr<sup>3+</sup> sites. EPR Spectra for bare MIL-101(Cr) matched the literature well and on binding of the imidazole to the Cr<sup>3+</sup> sites, broadening of the resonance signals is observed.3 Further analysis will be conducted by x-ray absorption spectroscopy (XAS) and Fourier transform infrared spectroscopy (FT-IR).<br/><br/>For the reaction of 1,2-epoxybutane with CO<sub>2</sub>, high activities were observed for all catalysts, achieving 80% conversion with 99% selectivity in 90 minutes. Complete conversion of the epoxide was reached after 6 hours.It is evident that when the imidazoles are heterogenised within the MIL-101 structure, the catalytic ability is greatly enhanced, with a highest turnover frequency (TOF) of 750 hr<sup>-1</sup> achieved.<br/><br/>Imidazole grafted MIL-101(Cr) has been shown to be a promising catalyst for the transformation of CO<sub>2</sub> to cyclic carbonates. Combing the absorptive, high surface area properties of MOFs with a targeted organic moiety, we have demonstrated the ability to produce a stable heterogeneous catalyst capable of high catalytic turnovers for CO<sub>2</sub> utilisation.<br/>