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BTU
Microscopic and spectroscopic characterization of interfaces and dielectric layers for OFET devices
(2009)
In this contribution we report on investigations of the electronic structure and composition of regioregular poly(3-hexylthiophene) (P3HT) and phenyl-C61-butyric acid methyl ester (PCBM) based films by using Near Edge X-Ray Absorption Fine Structure (NEXAFS). The measurements were done at the U49/2-PGM2 beam line of BESSY II, Berlin using TEY (total electron yield) and TFY (total fluorescence yield) detection. The samples were produced by spin casting a mixture of P3HT (dissolved in chloroform) and PCBM (dissolved in chlorobenzene) on ITO (indium tin oxide) coated glass slides. Measurements of pure P3HT and PCBM show all typical excitations, whereas the blended system is a weighted superposition of the related peaks. Analyzing these weighted superposition, we observe in the surface sensitive TEY data an accumulation of P3HT, whereas in the bulk sensitive TFY signal an as expected mixture is found. We also show angular dependent NEXAFS measurements of the P3HT/PCBM blend in order to measure the orientation and distribution of the P3HT polymer. Additionally, we will show a new approach for organic solar cell application by introducing ferroelectric nanoparticles into the mixture.
We use resonant photoemission at the C1s edge to study the
electronic structure of HOPG, graphene flakes and monolayer
graphene. We find remarkable differences in the profile of the Auger decay channels, which we attribute to an additional multiple-Auger with a three-hole final state. A prerequisite for the
appearance of this decay mechanism is the existence of localized excitonic states, which cause the appearance of the multiple Auger decay. We use those effects to identify the existence and the quantity of such defect states within the π*-band regime in carbon thin films, because the intensity of the three-hole Auger decay is varying with the defect density of the carbon films. We find that the appearance of the multiple Auger decay is different for multilayer and monolayer graphene. In particular the interaction of
impurities leads to broadening of the C1s core levels. The three-hole Auger decay spectroscopy is a new method to detect such
contaminations with a high sensitivity.
We use resonant photoemission at the C1s edge to study the electronic structure of HOPG, graphene flakes and monolayer graphene. We find remarkable differences in the profile of the Auger decay channels, which we attribute to an additional multiple-Auger with a three-hole final
state. A prerequisite for the appearance of this decay mechanism is the existence of localized excitonic states, which cause the appearance of the multiple Auger decay. Defects (pits, holes, steps and kinks) can act as localized excitonic states. We use those effects to identify the existence and the quantity of such defect states within the pi*-band regime in carbon thin films, because the intensity of the three-hole Auger decay is varying with the defect density of the carbon films.
The defect-excitonic states can be either localized in the band-gap at the M-point or in case of surface defects like steps, kinks or pits even at the K-point by losing the pure sp2 character of the films. We find that the appearance of the multiple Auger decay is different for multilayer and monolayer graphene. In particular the interaction of impurities leads to broadening of the C1s core levels. The three-hole Auger decay spectroscopy is a new method to detect such contaminations with a high sensitivity.
Spectroscopic characterization of Cobalt–Phthalocyanine electrocatalysts for fuel cell applications
(2012)
For polymer–electrolyte–membrane fuel cells (PEM-FC), platinumcatalysts on carbon based substrates are state
of the art, due to high electrochemical activity and chemical stability in acid electrolytes. High costs of platinum force investigations of alternative catalysts. With respect to the oxygen reduction reaction, possible candidates are transition metal (TM) complexes like TM-porphyrines or TM-phthalocyanines. Pyrolysis on carbon based substrates improves the catalytic activity. Highest activities were found for Fe or Co as transition metal centers. We present results of the pyrolysis of Co-phthalocyanine (CoPc) on carbon black. Besides an investigation of morphology by scanning electron microscopy (SEM) and chemical composition by energy dispersive X-ray spectroscopy (EDX) and X-ray photoelectron spectroscopy (XPS) during pyrolysis, we present a near edge X-ray absorption fine structure (NEXAFS) study of the chemical composition for the related annealing steps. This investigation is accompanied by an electrochemical characterization of the catalytic activity and selectivity. The XPS and NEXAFS data indicate a decomposition of the CoN4(chelate-) complex during pyrolysis. The N1s data for 800 °C show graphite-like, formally pyrrolic and pyridinic like features, without any significant contri-bution of Co. The Co2p data for both, XPS and NEXAFS are dominated by CoO/Co2O3. It can be concluded that during the pyrolysis cobalt particles are formed by the disintegration of CoN4-centers, after pyrolysis these par-ticles become oxidized upon contact with air.
Increasing green house emissions amplify global warming concerns worldwide. Fuel cells, based on polymer electrolyte membranes (PEM) are part of the solution to this issue. We aim at developing and testing new catalysts for fuel cells. Platinum catalysts perform best in PEM fuel cells to date but they are very expensive. For fuel cells to be perfectly applicable and economically affordable, an alternative catalyst with similar or even greater efficiency should be developed.
Metal phthalocyanines are known to be good oxygen reduction catalysts and are associated with high electron transfer properties. We investigated Cobalt Phthalocyanine in its pure state mixed with Carbon Black (CoPc:Carbon Black=1:9) untreated and also after a treatment in N2 at several temperatures, up to 1000°C for 30 minutes.
Results of XPS and EDX analyses reveal that the treatment at higher temperatures causes a rearrangement in the chemical states of Co, N and C atoms. Furthermore, results of cycling voltammetry (CV) analysis reveal that CoPc treated in N2 at 800°C exhibited a higher current density, in conclusion, a higher catalytic activity than the untreated CoPc.