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@PHDTHESIS{Grabowski:1024836,
author = {Grabowski, Frédéric},
othercontributors = {Pich, Andrij and Herres-Pawlis, Sonja},
title = {{C}ompartmentalized catalytically active microgels with
copper $\&$ zinc complexes},
school = {RWTH Aachen University},
type = {Dissertation},
address = {Aachen},
publisher = {RWTH Aachen University},
reportid = {RWTH-2026-00359},
pages = {1 Online-Ressource : Illustrationen},
year = {2025},
note = {Veröffentlicht auf dem Publikationsserver der RWTH Aachen
University 2026; Dissertation, RWTH Aachen University, 2025},
abstract = {The development of suitable carrier systems for catalysts
represents a significant challenge. In particular, the
compartmentalization of transition metal-complexes, which
belong to the type of homogeneous catalysts and are
dissolved in liquids, is of great interest in order to
improve chemical reactions in terms of controllability and
recyclability. Therefore, modern polymer science is focusing
on the immobilization of catalysts on responsive polymer
materials. These include microgels, which are
three-dimensional crosslinked, porous, soft, and mainly
spherical polymer colloids. Microgels exhibit responsive
properties to external stimuli, such as temperature, that
can additionally be used to control catalytic reactions. The
present Thesis focuses on the compartmentalization of
different transition metal-complexes into responsive
microgels for the application as catalytic carrier systems.
First, the microgel morphology is influenced by localization
of different pyrazolyl-modified monomers, which are
pre-selected by computer-guided simulations to obtain
anisotropic microgels. Subsequently, the synthesized
pyrazolyl-modified microgels are loaded with copper(II) to
form the corresponding complex in the microgel. By comparing
and combining analytical methods from the copper(II)
complexation studies of the pyrazolyl-modified monomers with
the microgels, the predominant complex within the microgels
is identified. The catalytic performance of the
copper(II)-pyrazolyl-complex modified microgels is
investigated regarding the morphology, localization, and
contents of the complex in the microgel in nitroaldol
(Henry) reactions. Afterwards, the best performing catalytic
microgel is used in an up-scaled continuous Henry reaction
for multiple cycles. The gained insights are used to prepare
zinc(II)-guanidine-complex modified microgels. For this
purpose, optimization reactions are carried out for the
synthesis of guanidine-modified microgels. The resulting
guanidine-modified microgels are in part loaded with
zinc(II). At the end, the zinc(II)-guanidine-complex
modified as well as the guanidine-modified microgels are
evaluated for their catalytic performance in the
depolymerization of polylactide and examined for their
recyclability. The Thesis shows that responsive microgels
are suitable carrier systems for various metalcomplexes,
enhancing their catalytic performance and recyclability.},
cin = {157010 / 150000},
ddc = {540},
cid = {$I:(DE-82)157010_20210903$ / $I:(DE-82)150000_20140620$},
pnm = {Funktionelle Mikrogele und Mikrogelsysteme
(FUNKTI-MIKROG-20170406) / SFB 985 C06 - Modulare,
kolloidale Katalysatoren basierend auf reaktiven Mikrogelen
(Mikrogelzyme) (C06) (317494828) / SFB 985 MGK -
Integriertes Graduiertenkolleg (MGK) (MGK) (221490978) /
Doktorandenprogramm / SFB 985: Funktionelle Mikrogele und
Mikrogelsysteme},
pid = {G:(DE-Juel1)FUNKTI-MIKROG-20170406 / G:(GEPRIS)317494828 /
G:(GEPRIS)221490978 / G:(DE-HGF)PHD-PROGRAM-20170404 /
G:(GEPRIS)191948804},
typ = {PUB:(DE-HGF)11},
doi = {10.18154/RWTH-2026-00359},
url = {https://publications.rwth-aachen.de/record/1024836},
}
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