Hydrogel-Embedded Model Photocatalytic System Investigated by Raman and IR Spectroscopy Assisted by Density Functional Theory Calculations and Two-Dimensional Correlation Analysis,The Journal of Physical Chemistry A

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Hydrogel-Embedded Model Photocatalytic System Investigated by Raman and IR Spectroscopy Assisted by Density Functional Theory Calculations and Two-Dimensional Correlation Analysis
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2018-02-26 00:00:00 , DOI: 10.1021/acs.jpca.7b12648
Robert Geitner ₁ , Stefan Götz _{2,

3} , Robert Stach ₄ , Michael Siegmann ₁ , Patrick Krebs ₄ , Stefan Zechel _{2,

3} , Kristin Schreyer _{2,

3} , Andreas Winter _{2,

3} , Martin D. Hager _{2,

3} , Ulrich S. Schubert _{2,

3} , Stefanie Gräfe ₁ , Benjamin Dietzek _{1,

5} , Boris Mizaikoff ₄ , Michael Schmitt ₁ , Jürgen Popp _{1,

3,

5}

Affiliation

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 C═N 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 C═N 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.

中文翻译：

密度泛函理论计算和二维相关分析辅助的拉曼和红外光谱研究的水凝胶包埋模型光催化体系

提出的研究报告了不同基质嵌入模型光催化剂的合成和振动光谱表征。该研究的目的是研究聚合物基质与光敏染料和金属配合物之间的相互作用，以用于潜在的未来光催化应用。合成的重点是新的若丹明B衍生物和Pt（II）吡啶吡啶配合物，它们均包含可聚合的甲基丙烯酸酯部分和酸不稳定的酰基hydr基团。甲基丙烯酸酯部分随后用于合成主要由聚（乙二醇）甲基丙烯酸酯单元组成的功能模型水凝胶。借助密度泛函理论计算和二维相关光谱技术的拉曼光谱和红外光谱研究了水凝胶的pH依赖性和温度依赖性行为。光谱结果表明，通过在酸性环境中裂解C═N键，可以从聚合物基质中释放出Pt（II）联吡啶复合物。尽管若丹明B染料具有可比的C═N键，但无法观察到相同的行为。温度相关的研究表明，水的蒸发既不影响水凝胶的分子结构，也不影响模型的光催化部分。尽管若丹明B染料具有可比的C═N键，但无法观察到相同的行为。温度相关的研究表明，水的蒸发既不影响水凝胶的分子结构，也不影响模型的光催化部分。尽管若丹明B染料具有可比的C═N键，但无法观察到相同的行为。温度相关的研究表明，水的蒸发既不影响水凝胶的分子结构，也不影响模型的光催化部分。

更新日期：2018-02-26

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