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@PHDTHESIS{Spitzner:994433,
author = {Spitzner, Robin},
othercontributors = {Klankermayer, Jürgen and Oppel, Iris Marga},
title = {{M}aßgeschneiderte molekulare {K}atalysatoren auf
{C}yclohexylbasis und {R}eaktionskonzepte für die {N}utzung
von $\mathrm{{CO}_{2}}$ als {C}1-{B}austein},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Aachen},
publisher = {RWTH Aachen University},
reportid = {RWTH-2024-09269},
pages = {1 Online-Ressource : Illustrationen},
year = {2024},
note = {Veröffentlicht auf dem Publikationsserver der RWTH Aachen
University; Dissertation, RWTH Aachen University, 2024},
abstract = {This thesis deals with the development of reaction concepts
and catalyst systems based on ruthenium and novel tripodal
cyclohexylligands for the partial reduction of CO2 with
molecular hydrogen. In the first chapter, a short
introduction is given and the current situation of different
economic sectors with regard to their CO2 emissions in the
EU is examined in detail. The usage of CO2 as a C1 building
block is identified as a possible approach for the
sustainable transformation of the current fossil-based
industry and the economic constraints and chemical
challenges are discussed. Finally, the objective and
structure of this thesis are presented. The second chapter
deals with the synthesis and characterisation of catalyst
structures based on tripodal cyclohexylligands and their
ruthenium complexes. This novel lead structure will be
investigated by varying the ligand backbone through the
introduction of functional groups with different properties,
so that structure-activity relationships of the catalysts
can be revealed and discussed. In Chapter 3, the synthesised
ruthenium complexes of the cyclohexylligands are used in the
catalytic hydrogenation of CO2 to various products. In
detail, the synthesis of dialkoxymethane, cyclic and linear
acetals and finally the production of methanol are
investigated in the order of the oxidation level of the
central carbon atom. The cyclohexylbased catalysts are
compared with the current state of the art based on
important key values in selected transformations of CO2.
Chapter 4 deals with the development of an immobilisation
and recycling strategy for the catalyst system presented.
The immobilisation of catalysts on solid polymer-based acid
supports is investigated. This type of immobilisation is
used in the synthesis of dimethoxymethane, cyclic and linear
acetals and methanol. In detail, a so-called ionomer (Nafion
NR50) is used for this purpose, which fulfils important
requirements for easy separation and recyclability due to
its interesting specific properties such as high Brönsted
acidity, Lewis acidity and high stability.},
cin = {154310 / 150000},
ddc = {540},
cid = {$I:(DE-82)154310_20190725$ / $I:(DE-82)150000_20140620$},
pnm = {BMBF 03SF0566P0 - Verbundvorhaben NAMOSYN
(BMBF-03SF0566P0)},
pid = {G:(DE-82)BMBF-03SF0566P0},
typ = {PUB:(DE-HGF)11},
doi = {10.18154/RWTH-2024-09269},
url = {https://publications.rwth-aachen.de/record/994433},
}
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