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  Rattle-type Catalysts with Spatially Distinct Active Centers for the Cascaded Valorization of Glucose

Joshi, H. (2020). Rattle-type Catalysts with Spatially Distinct Active Centers for the Cascaded Valorization of Glucose. PhD Thesis, Ruhr-Universität, Bochum.

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 Creators:
Joshi, Hrishikesh1, Author              
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1Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              

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 Abstract: Materials that enable tandem transformations offer substantial advantages in catalysis by reducing the number of separation steps. Typical examples are rattle-type materials that provide spatial isolation of matter and confinement of active centers which may favor the implementation of sequential catalytic cycles. However, the controlled synthesis of these solid catalysts suffers from several limitations. Therefore, the first part of the thesis addresses this aspect by studying the influence of various parameters in the synthesis of these materials including advanced oxidative methods such as gas- phase ozone treatment. In this first part, the synthesis is targeted at the development of catalysts for liquid phase transformation of glucose to furan derivatives such as HMF and FDCA. Liquid phase mass-transfer properties of rattle-type materials (e.g. diffusion constants) provide vital insight into their reactivity, especially for sequential reactions. However, obtaining diffusion constants within these materials under relevant reaction conditions is not easy. To this end, the second part of the thesis deals with the development of setups for these measurements in the liquid and gas phases. Breakthrough curves or uptake curves obtained from the experiments are fitted by an iterative simulation of the diffusion-advection equations via MATLAB. The best fit provides the required diffusion constants which can be correlated to the activity of catalysts. Therefore, the implementation of the solution and the development of the setup are major aspects of the second section of the thesis. The third part of the thesis deals with establishing a synergy between the three sequential reactions for the cascaded transformation of glucose to FDCA. This is attempted by modifying the hierarchical catalysts (rattle-type catalysts) with the required properties. The entire reaction scheme involves isomerization, dehydration and oxidation steps. A moderate-throughput approach is used to screen various hybrid materials and the reaction parameters to obtain the desired yield and selectivity. Overall, the impact of the thesis in the field of catalysis is to formulate a strategy towards the synthesis of rattle-type catalysts and the development of catalytic systems for tandem transformations with special focus on mass transfer properties.

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Language(s): eng - English
 Dates: 2020-04-222020-04-22
 Publication Status: Published in print
 Pages: 239
 Publishing info: Bochum : Ruhr-Universität
 Table of Contents: -
 Rev. Type: -
 Identifiers: -
 Degree: PhD

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