Hydrogel-Embedded Model Photocatalytic System Investigated by Raman and IR Spectroscopy Assisted by Density Functional Theory Calculations and Two-Dimensional Correlation Analysis
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Geitner, Robert; Goetz, Stefan; Stach, Robert; Siegmann, Michael; Krebs, Patrick; Zechel, Stefan; Schreyer, Kristin; Winter, Andreas; Hager, Martin D.; Schubert, Ulrich S.; Graefe, Stefanie; Dietzek, Benjamin; Mizaikoff, Boris; Schmitt, Michael; Popp, Juergen
- Abstract:
- The presented study reports the synthesis and
the vibrational spectroscopic characterization of different
matrix-embedded model photocatalysts. The goal of the study
is to investigate the interaction of a polymer matrix with
photosensitizing dyes and metal complexes for potential future
photocatalytic applications. The synthesis focuses on a new
rhodamine B derivate and a Pt(II) terpyridine complex, which
both contain a polymerizable methacrylate moiety and an acid
labile acylhydrazone group. The methacrylate moieties are
afterward utilized to synthesize functional model hydrogels
mainly consisting of poly(ethylene glycol) methacrylate units.
The pH-dependent and temperature-dependent behavior of the
hydrogels is investigated by means of Raman and IR
spectroscopy assisted by density functional theory calculations and two-dimensional correlation spectroscopy. The spectroscopic
results reveal that the Pt(II) terpyridine complex can be released from the polymer matrix by cleaving the CN bond in an acid
environment. The same behavior could not be observed in the case of the rhodamine B dye although it features a comparable
CN bond. The temperature-dependent study shows that the water evaporation has a significant influence neither on the
molecular structure of the hydrogel nor on the model photocatalytic moieties.
- Research areas:
- Year:
- 2018
- Type of Publication:
- Article
- Journal:
- Journal of Physical Chemistry A
- Volume:
- 122
- Pages:
- 2677 - 2687
- DOI:
- 10.1021/acs.jpca.7b12648