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Attaching photochemically active ruthenium polypyridyl complex units to amorphous hydrogenated carbon (a-C:H) layers

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Abstract
Amorphous hydrogenated carbon (a-C:H) films are applied 500 nm thick on Si(100) via plasma-enhanced chemical vapor deposition (PECVD) using ethyne. Present plasma conditions enrich the sp(2)-content especially toward the outermost a-C:H layers, which in turn are used to attach a photoactive Ru-polypyridyl complex to the surface. An azo-bridged dinuclear Ru-polypyridyl complex is optimized in synthesis and the final mononuclear fragment attached on a-C:H photochemically under UV-irradiation with concomitant N-2 release. The Ru-polypyridyl complex is characterized by MS, NMR, IR, UV/vis, fluorescence spectroscopy, and time-dependent density functional theory (DFT) calculations. Crystallographic data for the intermediate 4-nitro-2-(pyridin-2-yl)pyridine 1-oxide as essential precursor are established. Morphological characteristics of the a-C:H @ Si and final Ru(complex) @ a-C:H @ Si combinations are determined by atomic force microscopy (AFM) revealing individual grain-like structures. The presence of Ru on the a-C:H @ Si surface is initially verified qualitatively by laser-induced breakdown spectroscopy (LIBS) and by inductively coupled plasma-sector field mass spectrometry (ICP-SF-MS) after chemical digestion. With laser ablation-ICP-MS mapping, full Ru coverage is proven, also revealing inhomogeneities in terms of "Ru hot spots". The current investigation proves the successful attachment of a Ru-complex on a-C:H and indicates a starting point for the development of further material combinations for feasible sunlight to energy conversions.
Keywords
diamond-like carbon coating, ICP-MS mapping, laser-induced breakdown spectroscopy, ruthenium hot spots, surface morphology, DIAMOND-LIKE CARBON, DLC FILMS, TRIBOLOGICAL PROPERTIES, COATINGS, SURFACES, FUNCTIONALIZATION, IMMOBILIZATION, DEPOSITIONS, EVOLUTION, HISTORY

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Citation

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MLA
Schink, Carina et al. “Attaching Photochemically Active Ruthenium Polypyridyl Complex Units to Amorphous Hydrogenated Carbon (a-C:H) Layers.” ADVANCED MATERIALS INTERFACES 6.2 (2019): n. pag. Print.
APA
Schink, C., Catena, A., Heintz, K., Görls, H., Beresko, C., Ankerhold, G., von der Au, M., et al. (2019). Attaching photochemically active ruthenium polypyridyl complex units to amorphous hydrogenated carbon (a-C:H) layers. ADVANCED MATERIALS INTERFACES, 6(2).
Chicago author-date
Schink, Carina, Alberto Catena, Katharina Heintz, Helmar Görls, Christian Beresko, Georg Ankerhold, Marcus von der Au, et al. 2019. “Attaching Photochemically Active Ruthenium Polypyridyl Complex Units to Amorphous Hydrogenated Carbon (a-C:H) Layers.” Advanced Materials Interfaces 6 (2).
Chicago author-date (all authors)
Schink, Carina, Alberto Catena, Katharina Heintz, Helmar Görls, Christian Beresko, Georg Ankerhold, Marcus von der Au, Björn Meermann, Stijn Van Malderen, Frank Vanhaecke, Stefan Wehner, Wolfgang Imhof, and Christian B Fischer. 2019. “Attaching Photochemically Active Ruthenium Polypyridyl Complex Units to Amorphous Hydrogenated Carbon (a-C:H) Layers.” Advanced Materials Interfaces 6 (2).
Vancouver
1.
Schink C, Catena A, Heintz K, Görls H, Beresko C, Ankerhold G, et al. Attaching photochemically active ruthenium polypyridyl complex units to amorphous hydrogenated carbon (a-C:H) layers. ADVANCED MATERIALS INTERFACES. 2019;6(2).
IEEE
[1]
C. Schink et al., “Attaching photochemically active ruthenium polypyridyl complex units to amorphous hydrogenated carbon (a-C:H) layers,” ADVANCED MATERIALS INTERFACES, vol. 6, no. 2, 2019.
@article{8586881,
  abstract     = {Amorphous hydrogenated carbon (a-C:H) films are applied 500 nm thick on Si(100) via plasma-enhanced chemical vapor deposition (PECVD) using ethyne. Present plasma conditions enrich the sp(2)-content especially toward the outermost a-C:H layers, which in turn are used to attach a photoactive Ru-polypyridyl complex to the surface. An azo-bridged dinuclear Ru-polypyridyl complex is optimized in synthesis and the final mononuclear fragment attached on a-C:H photochemically under UV-irradiation with concomitant N-2 release. The Ru-polypyridyl complex is characterized by MS, NMR, IR, UV/vis, fluorescence spectroscopy, and time-dependent density functional theory (DFT) calculations. Crystallographic data for the intermediate 4-nitro-2-(pyridin-2-yl)pyridine 1-oxide as essential precursor are established. Morphological characteristics of the a-C:H @ Si and final Ru(complex) @ a-C:H @ Si combinations are determined by atomic force microscopy (AFM) revealing individual grain-like structures. The presence of Ru on the a-C:H @ Si surface is initially verified qualitatively by laser-induced breakdown spectroscopy (LIBS) and by inductively coupled plasma-sector field mass spectrometry (ICP-SF-MS) after chemical digestion. With laser ablation-ICP-MS mapping, full Ru coverage is proven, also revealing inhomogeneities in terms of "Ru hot spots". The current investigation proves the successful attachment of a Ru-complex on a-C:H and indicates a starting point for the development of further material combinations for feasible sunlight to energy conversions.},
  articleno    = {1801308},
  author       = {Schink, Carina and Catena, Alberto and Heintz, Katharina and Görls, Helmar and Beresko, Christian and Ankerhold, Georg and von der Au, Marcus and Meermann, Björn and Van Malderen, Stijn and Vanhaecke, Frank and Wehner, Stefan and Imhof, Wolfgang and Fischer, Christian B},
  issn         = {2196-7350},
  journal      = {ADVANCED MATERIALS INTERFACES},
  keywords     = {diamond-like carbon coating,ICP-MS mapping,laser-induced breakdown spectroscopy,ruthenium hot spots,surface morphology,DIAMOND-LIKE CARBON,DLC FILMS,TRIBOLOGICAL PROPERTIES,COATINGS,SURFACES,FUNCTIONALIZATION,IMMOBILIZATION,DEPOSITIONS,EVOLUTION,HISTORY},
  number       = {2},
  pages        = {11},
  title        = {Attaching photochemically active ruthenium polypyridyl complex units to amorphous hydrogenated carbon (a-C:H) layers},
  url          = {http://dx.doi.org/10.1002/admi.201801308},
  volume       = {6},
  year         = {2019},
}

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