PubMed · 6407862
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I Rosenthal. 1983-07-15. A working hypothesis for negative ion generators.. https://doi.org/10.1007/bf01990289
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The internal energy distributions, P(epsilon), of a millisecond pulsed radio frequency glow discharge plasma were investigated using tungsten hexcarbonyl W(CO)(6) as a "thermometer molecule". Vapor of the probe molecule, W(CO)(6), was introduced into the plasma and subjected to various ionization and excitation processes therein. The resultant molecular and fragment ions were monitored using a Time-of-Flight mass spectrometer. Ion abundance data were utilized in combination with the known energetics of W(CO)(6) to construct the P(epsilon) plots. The P(epsilon) of W(CO)(6) exhibited strong temporal dependence over the pulse cycle: Distinct internal energy distributions were found at the discharge breakdown period (prepeak), the steady state period (plateau), and the post-pulse period (afterpeak). Spatial variation in P(epsilon) was also observed, especially during the plateau regime. The observations suggest that this pulsed glow discharge affords excellent energy tunability that can be used to perform selective ionization and fragmentation for molecular, structural, and elemental information. Parametric studies were performed to evaluate the effects of discharge pressure and operating power on P(epsilon). These studies also provided insight into the correlation of the observed P(epsilon)s with the fundamental ionization and excitation mechanisms in the plasma. The temporal and spatial variations in P(epsilon) were hence attributed to changes in the dominant energy transfer processes at specific times in specific regions of the plasma. These data will be useful in future efforts to optimize the analytical performance of this source for chemical speciation.
A kinetic model is developed for the dynamic events occurring within an atmospheric sampling glow discharge that affect its performance as an ion source for analytical mass spectrometry. The differential equations incorporate secondary electron generation and thermalization, reagent and analyte ion formation via electron capture and ion-molecule reactions, ion loss via recombination processes, diffusion, and ion-molecule reactions with matrix components, and the sampling and pumping parameters of the source. Because the ion source has a flow-through configuration, the number densities of selected species can be estimated by applying the steady-state assumption. However, understanding of its operation is aided by knowledge of the dynamic behavior, so numerical methods are applied to examine the time dependence of those species as well. As in other plasma ionization sources, the ionization efficiency is essentially determined by the ratio of the relevant ion formation and recombination rates. Although thermal electron and positive reagent ion number densities are comparable, the electron capture/ion-molecule reaction rate coefficient ratio is normally quite large and the ion-electron recombination rate coefficient is about an order of magnitude greater than that for ion-ion recombination. Consequently, the efficiency for negative analyte ion formation via electron capture is generally superior to that for positive analyte ion generation via ion-molecule reaction. However, the efficiency for positive analyte ion formation should be equal to or better than that for negative analyte ions when both ionization processes occur via ion-molecule reaction processes (with comparable rate coefficients), since the negative reagent ion density is considerably less than that for positive reagent ions. Furthermore, the particularly high number densities of thermal electrons and reagent ions leads to a large dynamic range of linear response for the source. Simulation results also suggest that analyte ion number densities might be enhanced by modification of the standard physical and operating parameters of the source.
The degradation of methamidophos in pure bi-distilled water (with initial concentration 5 mg L(-1), pH = 7 at the beginning) was studied. For the first time, 2 ionised air water treatment pilot systems (IAPS-1, -2, no additives) were set up (Figs. 1 and 2). The degradation of methamidophos was carried out with only the IAPS-2 and with two different ultraviolet (UV) lamps: high- and low-pressure mercury lamps (HP and LP, with or without H202). The kinetics of these oxidative processes was investigated. The highest rate constant was reached by the LP, 0.2% H2O2 (k = 0.7524min(-1), t 1/2 = 0.9min), followed closely by both treatments with the HP, 0.2% H202 (k = 0.6328min(-1), t 1/2 = 1.1 min) and LP, 0% H202 (k = 0.4749min(-1), t 1/2 = 1.5 min). The lowest rate constants were achieved from the HP, 0% H202 process (k = 0.0303min(-1), t 1/2 = 22.9min) and from the IAPS-2 (k = 0.0117 min(-1), t 1/2 = 59.2min). The mineralisation of methamidophos was confirmed by the determination of the anions produced including NO3-, PO4(3-) and SO4(2-) during and at the end of each experiment. The toxicity of water samples before, during and after the experiments was tested with Daphnia test.