Recently, more attention both in research and industry fields is focused on the development of new environmental-friendly technologies which reduce or eliminate the use or generation of hazardous substances. Catalysis represents a useful tool to perform this task as it is able to promote alternative less energy demanding reaction paths leading thus to milder conditions. In this Thesis work, carried out as part of a scientific collaboration thanks to an Erasmus agreement between the University of Turin (IT) and the University of Southampton (UK), a new family of heterogeneous catalysts based on noble metal nanoparticles supported by copper chloropyrophosphate frameworks (CuClP) has been synthesised. A novel hydrothermal procedure and subsequent thermal activations were adopted. Several samples, both monometallic (Au/CuClP, Pt/CuClP) and bimetallic (AuPt/CuClP) have been prepared with 7 % wt of metal loading. Particularly, various AuPt/CuClP catalysts by changing the ratio among Au and Pt were obtained. During the first part of this work, a conventional activation procedure was employed by conventionally heating the samples under a reductant flow. Later, using microwave-assisted heating successful activation results were obtained by drastically reducing the process time. The catalytic activity has been tested successfully for the solvent-free selective aerobic oxidation of KA-oil, a mixture made up of cyclohexanol and cyclohexanone which is industrially produced by the oxidation of cyclohexane. During the first part of this work, the catalytic tests were carried out using a continuous-flow reactor whereas later, some preliminary experiments to reproduce analogous results using microwave-assisted heating were performed. Lastly, various characterisation techniques among which PXRD, DR UV-Vis and HRTEM on as-synthesised, activated and used catalysts have been carried out.

Nanoparticelle bimetalliche estruse da framework CuClP per processi Green.

GRASSO, SARAH
2016/2017

Abstract

Recently, more attention both in research and industry fields is focused on the development of new environmental-friendly technologies which reduce or eliminate the use or generation of hazardous substances. Catalysis represents a useful tool to perform this task as it is able to promote alternative less energy demanding reaction paths leading thus to milder conditions. In this Thesis work, carried out as part of a scientific collaboration thanks to an Erasmus agreement between the University of Turin (IT) and the University of Southampton (UK), a new family of heterogeneous catalysts based on noble metal nanoparticles supported by copper chloropyrophosphate frameworks (CuClP) has been synthesised. A novel hydrothermal procedure and subsequent thermal activations were adopted. Several samples, both monometallic (Au/CuClP, Pt/CuClP) and bimetallic (AuPt/CuClP) have been prepared with 7 % wt of metal loading. Particularly, various AuPt/CuClP catalysts by changing the ratio among Au and Pt were obtained. During the first part of this work, a conventional activation procedure was employed by conventionally heating the samples under a reductant flow. Later, using microwave-assisted heating successful activation results were obtained by drastically reducing the process time. The catalytic activity has been tested successfully for the solvent-free selective aerobic oxidation of KA-oil, a mixture made up of cyclohexanol and cyclohexanone which is industrially produced by the oxidation of cyclohexane. During the first part of this work, the catalytic tests were carried out using a continuous-flow reactor whereas later, some preliminary experiments to reproduce analogous results using microwave-assisted heating were performed. Lastly, various characterisation techniques among which PXRD, DR UV-Vis and HRTEM on as-synthesised, activated and used catalysts have been carried out.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.14240/49777