low frequency

Determination of NO densities in a surface dielectric barrier discharge using optical emission spectroscopy

A new computationally assisted diagnostic to measure NO densities in atmospheric-pressure microplasmas by Optical Emission Spectroscopy (OES) is developed and validated against absorption spectroscopy in a volume Dielectric Barrier Discharge (DBD). The OES method is then applied to a twin surface DBD operated in N2 to measure the NO density as a function of the O2 admixture (0:1%–1%). The underlying rate equation model reveals that NO(A2Σ+) is primarily excited by reactions of the ground state NO(X2Π) with metastables N2(A3Σ+u).

Publisher: 
AEPT
Project: 
SFB 1316
Authors: 
B. Offerhaus
F. Kogelheide
D. Jalat
N. Bibinov
J. Schulze
K. Stapelmann
P. Awakowicz

Intra-cavity dynamics in a microplasma channel by side-on imaging

Here, a microplasma channel was investigated. The setup consists of three stacked layers: a magnet, a dielectric foil and two nickel foils that are separated by a 120 μm wide gap. The magnet is grounded while the two nickel foils are powered. The setup was operated with a triangular voltage with a frequency of 10 kHz and an amplitude of up to 700 V in Helium at atmospheric pressure. Phase resolved emission images were used to investigate the microplasma channel dynamics with line of sight from the top and from the side to the inside of the cavity. The top view images revealed that the discharge in the microplasma channel and the microplasma arrays behave similar. The already known asymmetric discharge behavior, the self-pulsing and the wavelike ignition was also observed in the microplasma channel. For the wavelike ignition in the channel a simple one dimensional model was proposed. With the additional side view images the asymmetric discharge behavior was examined more thoroughly. Unlike in the microplasma arrays, the discharge expands here in both half periods of the applied voltage above the upper edge of the powered electrodes. The discharge extends over a larger width in the half period, in which the potential of the upper electrodes is increasing, while it extends over a larger height in the other half period. Phase resolved images were also used to investigate the ignition phase of the discharge. The discharge ignites in the two half periods on a different height. This was explained by modeling the drift and diffusion of the charged particles between two discharge pulses.

Publisher: 
EP2
Project: 
SFB 1316
Authors: 
S. Kreuznacht
M. Böke
V. Schulz-von der Gathen

Characterisation of volume and surface dielectric barrier discharges in N2–O2 mixtures using optical emission spectroscopy

A volume and a twin surface dielectric barrier discharge (VDBD and SDBD) are generated in different nitrogen–oxygen mixtures at atmospheric pressure by applying damped sinusoidal voltage waveforms with oscillation periods in the microsecond time scale. Both electrode configurations are located inside vacuum vessels and operated in a controlled atmosphere to exclude the influence of surrounding air. The discharges are characterised with different spatial and temporal resolution by applying absolutely calibrated optical emission spectroscopy in conjunction with numerical simulations and current–voltage measurements. Plasma parameters, namely the electron density and the reduced electric field, and the dissipated power are found to depend strongly on the oxygen content in the working gas mixture. Different spatial and temporal distributions of plasma parameters and dissipated power are explained by surface and residual volume charges for different O2 admixtures due to their effects on the electron recombination rate. Thus, the oxygen admixture is found to strongly influence the breakdown process and plasma conditions of a VDBD and a SDBD.

Publisher: 
AEPT
Project: 
SFB 1316
Authors: 
F. Kogelheide
B. Offerhaus
N. Bibinov
P. Krajinski
L. Schücke
J. Schulze
K. Stapelmann
P. Awakowicz

In-situ control of microdischarge characteristics in unipolar pulsed plasma electrolytic oxidation of aluminum

Microdischarges occurring during plasma electrolytic oxidation are the main mechanism promoting oxide growth compared to classical anodization. When the dissipated energy by microdischarges during the coating process gets too large, high-intensity discharges might occur, which are detrimental to the oxide layer. In bipolar pulsed plasma electrolytic oxidation a so called 'soft-sparking' mode limits microdischarge growth. This method is not available for unipolar pulsing and for all material combinations. In this work, the authors provide a method to control the size- and intensity distributions of microdischarges by utilizing a multivariable closed-loop control. In-situ detection of microdischarge properties by CCD-camera measurements and fast image processing algorithms are deployed. The visible size of microdischarges is controlled by adjusting the duty cycle in a closed-loop feedback scheme, utilizing a PI-controller. Uncontrolled measurements are compared to controlled cases. The microdischarge sizes are controlled to a mean value of A = 510^-3 mm^2 and A = 710^-3 mm^2, respectively. Results for controlled cases show, that size and intensity distributions remain constant over the processing time of 35 minutes. Larger, high-intensity discharges can be effectively prevented. Optical emission spectra reveal, that certain spectral lines can be influenced or controlled with this method. Calculated black body radiation fits with very good agreement to measured continuum emission spectra (T = 3200 K). Variance of microdischarge size, emission intensity and continuum radiation between consecutive measurements is reduced to a large extent, promoting uniform microdischarge and oxide layer properties. A reduced variance in surface defects can be seen in SEM measurements, after coating for 35 minutes, for controlled cases. Surface defect study shows increased number density of microdischarge impact regions, while at the same time reducing pancake diameters, implying reduced microdischarge energies compared to uncontrolled cases.

Publisher: 
AEPT
Project: 
SFB 1316
Authors: 
P. Hermanns
S. Böddeker
V. Bracht
N. Bibinov
P. Awakowicz

Plasma‐driven in situ production of hydrogen peroxide for biocatalysis

Peroxidases and peroxygenases are promising classes of enzymes for biocatalysis because of their ability to carry out one‐electron oxidation reactions and stereoselective oxyfunctionalizations. However, industrial application is limited, as the major drawback is the sensitivity toward the required peroxide substrates. Herein, we report a novel biocatalysis approach to circumvent this shortcoming: in situ production of H2O2 by dielectric barrier discharge plasma. The discharge plasma can be controlled to produce hydrogen peroxide at desired rates, yielding desired concentrations. Using horseradish peroxidase, it is demonstrated that hydrogen peroxide produced by plasma treatment can drive the enzymatic oxidation of model substrates. Fungal peroxygenase is then employed to convert ethylbenzene to (R)‐1‐phenylethanol with an ee of >96 % using plasma‐generated hydrogen peroxide. As direct treatment of the reaction solution with plasma results in reduced enzyme activity, the use of plasma‐treated liquid and protection strategies are investigated to increase total turnover. Technical plasmas present a noninvasive means to drive peroxide‐based biotransformations.

Publisher: 
Applied Microbiology
Project: 
SFB 1316
Authors: 
A. Yayci
A. Gomez Baraibar
M. Krewig
E. Fernandez Fueyo
F. Hollmann
M. Alcaide
R. Kourist
J. Bandow

Dielectric barrier discharge plasma treatment affects stability, metal ion coordination, and enzyme activity of bacterial superoxide dismutases

A molecular‐level understanding of the effects of atmospheric‐pressure plasma on biological samples requires knowledge of the effects on proteins. Superoxide dismutases, which detoxify superoxide under oxidative stress conditions, play a key role in bacterial plasma resistance. Investigation of the impact of dielectric barrier discharge (DBD) treatment on purified superoxide dismutases SodA and SodB of Escherichia coli showed that DBD treatment caused a rapid protein degradation, with only 8% of protein remaining after 10 min. The affinity of SodA for the metal cofactor Mn2+ was reduced. Mass spectrometry, in conjunction with coupled‐cluster calculations, revealed that modifications of amino acid residues in the active site can explain the decreased metal affinity and a distortion of the coordination geometry responsible for the activity loss.

Publisher: 
Applied Microbiology
Project: 
SFB 1316
Authors: 
M. Krewig
C. Jung
E. Dobbelstein
B. Schubert
T. Jacob
J. Bandow