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Diagnosis Of H3-/D3- Anions And OH Radicals In Non-Thermal Equilibrium Plasmas

Posted on:2009-07-17Degree:DoctorType:Dissertation
Country:ChinaCandidate:W C WangFull Text:PDF
GTID:1101360242484578Subject:Applied Chemistry
Abstract/Summary:PDF Full Text Request
Molecular-beam mass spectrometry (MBMS) and emission spectroscopy techniqueshave been used respectively to diagnose the H3-/D3- anions in hydrogen plasmas producedby dielectric barrier discharges and the OH radicals generated by pulsed corona discharge.The main results presented in the dissertation have been summarized as follows:1. H3- anions produced by pure hydrogen dielectric barrier discharges have beendiagnosed by the molecular beam mass spectrometry (MBMS) at gas pressure from 1.5to 7.6 Torr. The stability of H3- anions is further demonstrated experimentally by theexperiments using hydrogen's isotope deuterium. The signal intensity rate of H3-/H- ishigher than that of the controversial experimental results reported earlier by six ordersof magnitude, and the lifetimes of the H3- and D3- anions observed in our experimentsare greater than 50μs and 70μs respectively. The possible mechanism of forming H3-anions by three-body collisions (H-+ H2 + M→H3-+ M) is proposed for the first time. The observed results confirmed the stability of H3-. The consistent conclusion of the stability of H3- anions in theory and experiment is obtained.The effects of gas pressure and discharge parameters on the ion currents of H3-/H-have been investigated. The observed ion current of H- is one to several orders of magnitude higher than that of H3- at gas pressure from 1.5 to 7.6 Torr at 40 kV peak-peak discharge voltage and 35 kHz discharge frequency. Only H- ion signal is observed at gas pressure from 7.7 to 60 Torr. The ion current of H- increases with the increasing of discharge peak voltage and discharge frequency, and exhibits a maximum over the studied range of gas pressure.The effects of gas pressure, discharge peak voltage, and discharge frequency on the ion currents of positive ions (H+, H2+, and H3+) in cathode sheath region produced by dielectric barrier discharge hydrogen plasmas have been also investigated at gas pressure from 1.0 to 80 Torr.2. The emission spectra of OH(A2∑→X2Π, 0-0), O(3p5P→3s5S20) and H(n=3-2) produced by the positive pulsed corona discharge of N2 and H2O mixture in a needle-plate reactor have been successfully recorded against a severe electromagnetic interference coming from the pulsed corona discharge at one atmosphere. The relative populations and the vibrational temperature of N2 (C, v') were determined with the corresponding Franck-Condon factor and the emission intensities of theΔv=-3 andΔv=-4 vibration transition band of N2 (C3Πu→B3Πg). The emission intensity of OH (A2∑→X2Π0-0) can be obtained by subtracting the emission intensity of theΔv = +1 vibration transition band of N2 (C3Πu→B3Πg) from the overlapping spectra. The relative populations of OH (A2∑) and O(3p5P) have been obtained by the emission intensity of OH and O and the corresponding Einstein's transition probabilities. The effects of pulsed peak voltage, pulsed repetition rate, and oxygen flow on the emission intensities of OH (A2∑→X2Π0-0), O(3p5P→3s5S20 777.4 nm), H (n=3-2 656.3 nm) and the relative populations of OH (A 2) and O(3p P) are investigated.It is found that when the pulsed peak voltage and the pulsed repetition rate are increased, the emission intensities of OH (A2∑→X2Π0-0), O (3p5P→3s5S20 777.4 nm), and H (n=3-2 656.3 nm) enhance correspondingly. The emission intensities of O (3p5P→3s5S20 777.4 nm) and H (n=3-2 656.3 nm) increase with the flow rate of oxygen (from 0 to 30 ml/min) and achieve a maximum value at flow rate of 30 ml/min. When the flow rate of oxygen is increased further, the intensities decrease obviously. The emission intensity of OH (A2∑→X2Π0-0) decreases with the flow rate of oxygen. When the flow rate of oxygen increases from 0 to 30 ml/min, the relative population of O (3p5P) active atom increases and achieve a maximum value at flow rate of 30 ml/min. When the flow rate of oxygen is increased further, the relative population of O(3p5P) active atoms decreases obviously. And the relative population of OH(A2∑) radical decreases nonlinearly with the flow rate of oxygen.3. The emission spectra of OH (A2∑→X2Π0-0) and N2(C3Πu→B3Πg) produced by the bi-directional pulsed corona discharge of N2 and H2O mixture in a wire-plate reactor have been successfully recorded at one atmosphere. The relative populations and the vibrational temperature of N2 (C, v') and the emission intensity of OH (A2∑→X2Π0-0) are determined. The effects of pulsed peak voltage, pulsed repetition rate, and oxygen flow on the emission intensity of OH (A2∑→X2Π0-0) and the relative population of OH (A2∑) are investigated. It is found that the emission intensity of OH (A2∑→X2Π0-0) enhance correspondingly with increasing the pulsed peak voltage and the pulsed repetition rate. The relative population of OH (A2∑) rises linearly with increasing the pulsed peak voltage and the pulsed repetition rate. When the oxygen is added in N2 and H2O mixture gas, the emission intensity of the OH (A2∑→X2Π0-0) decreases rapidly. The relative population of OH (A2∑) radical decreases exponentially with increasing the added the flow rate of oxygen.
Keywords/Search Tags:Triatomic hydrogen anions, OH radicals, Dielectric barrier discharge, Pulsed corona discharge, Molecular beam mass spectrometry, Emission spectrometry
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