6 Materialchemie
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Structural changes of highly active Pd/MeOx (Me = Fe, Co, Ni) during catalytic methane combustion
(2018)
Fe2O3, Co3O4 and NiO nanoparticles were prepared via a citrate method and further functionalized with Pd by impregnation. The pure oxides as well as Pd/Fe2O3, Pd/Co3O4, and Pd/NiO (1, 5 and 10 wt % Pd) were employed for catalytic methane combustion under methane lean (1 vol %)/oxygen rich (18 vol %, balanced with nitrogen) conditions. Already, the pure metal oxides showed a high catalytic activity leading to complete conversion temperature of T100 ≤ 500 °C. H2-TPR (Temperature-programmed reduction) experiments revealed that Pd-functionalized metal oxides exhibited enhanced redox activity compared to the pure oxides leading to improved catalytic combustion activity at lower temperatures. At a loading of 1 wt % Pd, 1Pd/Co3O4 (T100 = 360 °C) outperforms 1Pd/Fe2O3 (T100 = 410 °C) as well as 1Pd/NiO (T100 = 380 °C). At a loading of 10 wt % Pd, T100 could only be slightly reduced in all cases. 1Pd/Co3O4 and 1Pd/NiO show reasonable stability over 70 h on stream at T100. XPS (X-ray photoelectron spectroscopy) and STEM (Scanning transmission electron microscopy) investigations revealed strong interactions between Pd and NiO as well as Co3O4, respectively, leading to dynamic transformations and reoxidation of Pd due to solid state reactions, which leads to the high long-term stability.
The passivation behavior of alloy 31 was investigated as a function of passivation potential in a green-death solution at 40 °C. The alloy 31 surface is in a stable passive state during cyclic potentiodynamic polarization. In potentiostatic polarization of alloy 31, passive current density increases with an increase in the passivation potential. Electrochemical impedance spectroscopy (EIS) and Mott–Schottky (M–S) analysis showed that a more defective n-type semiconductive passive film forms as the potential increases. X-ray photoelectron spectroscopy (XPS) revealed that passive film consists of mainly chromium and minor iron and nickel oxides. The increase of the applied potential is considered to be a reason for the change in passive film stability.
Thermoresponsive polymer coatings can facilitate cell sheet fabrication under mild conditions by promoting cell adhesion and proliferation at 37 1C. At lower temperatures the detachment of confluent cell sheets is triggered without enzymatic treatment. Thus, confluent cell sheets with intact extracellular matrix for regenerative medicine or tissue engineering applications become available. Herein, we applied the previously identified structural design parameters of functional, thermoresponsive poly(glycidyl ether) brushes on gold to the more application-relevant substrate glass via the self-assembly of a corresponding block copolymer (PGE-AA) with a short surface-reactive, amine-presenting anchor block. Both, physical and covalent immobilization on glass via either multivalent ionic interactions of the anchor block with bare glass or the coupling of the anchor block to a polydopamine (PDA) adhesion layer on glass resulted in stable coatings. Atomic force microscopy revealed a high degree of roughness of covalently attached coatings on the PDA adhesion layer, while physically attached coatings on bare glass were smooth and in the brush-like regime. Cell sheets of primary human dermal fibroblasts detached reliably (86%) and within 20 ± 10 min from physically tethered PGE-AA coatings on glass when prepared under cloud point grafting conditions. The presence of the laterally inhomogeneous PDA adhesion layer, however, hindered the spontaneous temperature-triggered cell detachment from covalently grafted PGE-AA, decreasing both detachment rate and reliability. Despite being only physically attached, self-assembled monolayer brushes of PGE-AA block copolymers on glass are functional and stable thermoresponsive coatings for application in cell sheet fabrication of human fibroblasts as determined by X-ray photoelectron spectroscopy.