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Interface assembled molecular aggregates materials and electrochemical studies

Author: LiuAn
Tutor: QianDongJin
School: Fudan University
Course: Inorganic Chemistry
Keywords: Molecular aggregates Interfacial Assembly Nano pore structure Hydrogenase Viologen
CLC: O631.3
Type: Master's thesis
Year: 2010
Downloads: 65
Quote: 0
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Abstract


Through non-covalent interactions between molecules form ordered molecular aggregates has increasingly become a molecular-level chemical research hotspot. Organic or inorganic small molecules, macromolecules, are macrocyclic molecules can be used as building blocks to build ordered molecular aggregates, thereby preparing new material and to achieve its catalytic, magnetic, optical, molecular devices, electrical, gas storage and other functions. Common methods include construction of gas - liquid interface Langmuir-Blodgett (LB) technique, self-assembly techniques, layer assembly technology. This work is divided into two parts. The first part of the work in order to force non-covalent molecular aggregates formed by chemical materials has increasingly become a hot research topic, in which the most interesting supramolecular chemistry. We selected six different pyridyl-containing compounds as polydentate ligands, the use of the interface assembly method, based on the metal ions and polydentate ligand coordination interaction between the successfully assembled on a solid substrate surface was six different types of coordination polymer multilayers. We study the spectral properties of the films and electrochemical properties. The results show that the size of the ligand affect the film properties, electrical activity of the Fe (CN) 63-/4- sodium ions can penetrate the pore structure matching the size with polymer multilayers. Studied in six ligands, BPy and PVP polymer multilayer film formed relatively dense, pore size is small, difficult to pass through the electro-active material, and TPyTa, Fe (pyterpy) 2, BNAPy, TPyP formation polymer multilayer membrane pore size larger electro-active substances can pass through cyclic voltammetry showed reversible or quasi-reversible redox peaks. Because of this coordination bond based on self-assembled film has good chemical and thermal stability, can be used to build a three-dimensional surface of the solid system of the main object, the film can also be used to study the electron or charge transfer process. The second part of the work, the hydrogen enzyme as a good biological catalyst, catalytic hydrogen oxidation and proton reduction obtained, for better achieve clean energy production and environmental protection is important. Catalase activity centers are generally buried in the center of the molecule, electron transfer and the catalytic reaction is very difficult, and it is very good viologen electron transfer mediator, we use a positively charged cations and negatively charged electrolyte between hydrogenase electrostatic interactions successfully assembled catalase - cation electrolyte composite membrane. We selected a group containing viologen and viologen group does not contain electrolytes as subphase in the air - water interface to obtain hydrogen enzyme molecule monolayers, due to the formation of polyelectrolyte subphase catalase - poly Purple fine complexes, the formed thin film becomes more hydrophobic, and molecules to occupy a greater area and surface pressure. Catalase and cationic polymer LB films formed after the active center of the enzyme molecule of hydrogen and the electrode surface to achieve electronic exchange. We further studied the transfer to the solid substrate catalase - viologen derivative composite film, the obtained results show that the composite film has good electrochemical and catalytic activity, which may be applied in the conversion of hydrogen, then in the biological production of hydrogen and biofuel cell has a potential application.

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CLC: > Mathematical sciences and chemical > Chemistry > Polymer chemistry ( polymer ) > Polymer physics and physical chemistry of polymers > The chemical nature of polymers
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