Štúdium chemických procesov v mimozemských atmosférach
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Vysoké učení technické v Brně. Fakulta chemická
Abstract
Cieľom predkladanej práce je štúdium chemických procesov v mimozemských atmosférach a syntéza organických zlúčenín vznikajúcich v elektrických výbojoch v plynnej zmesi. Táto štúdia je zameraná najmä na simuláciu atmosféry Titanu. Najčastejšie zloženie plynnej zmesi bolo metán (1-4 sccm) v 200 sccm dusíku. Prebiehali tiež merania so stopovým množstvom kyslíku a oxidu uhličitého. Okrem zloženia plynnej zmesi sa menila aj velkosť dodávaného elektrického výkonu od 2 W – 12 W. Merania prebiehali za laboratórnej teploty ale aj pri teplote kvapalného dusíka, čím sa experiment výrazne priblížil reálnym podmienkam na Titane. Identifikácia syntetizovaných plynných produktov v reaktore prebiehala väčšinou pomocou hmotnostnej spektrometrie s protónovou ionizáciou. Ďalej prebehli aj merania pomocou iónovej mobilnej spektrometrie a infračervenej spektrometrie s Fourierovou transformáciou. Samotný výboj bol charakterizovaný pomocou optickej emisnej spektrometrie, ktorá potvrdzuje prítomnosť aktívnych foriem dusíka a radikálov vznikajúcich z metánu. Okrem toho boli v nameraných spektrách identifikované aj prvý negatívny a druhý pozitívny systém dusíku a tiež fialový systém radikálu CN. Z druhého pozitívneho systému dusíka bola stanovená rotačná teplota na približnú hodnotu 2300-2400 K. Vibračná teplota bola stanovená tiež z tohto systému v závislosti na zložení plynnej zmesi od 3100-3400 K. Ďalej bola vibračná teplota vypočítaná z prvého negatívneho systému dusíka, ktorá ale s koncentráciou metánu mierne klesala a rástla s výkonom v intervale od 3950-4350 K. Veľmi podobnú závislosť mala aj vibračná teplota získaná pre fialový spektrálny systém CN, ktorej hodnota sa nachádzala v intervale od 5900 do 7700 K. Pomocou hmotnostného spektrometra s protónovou ionizáciou bolo detegovaných za laboratórnej teploty množstvo alifatických uhľovodíkov, niektoré aromatické uhľovodíky a tiež amino či kyano zlúčeniny. Najvyššie molekulové hmotnosti za laboratórnej teploty boli do 150 g.mol-1 pri čom najviac zastúpenými látkami boli kyanovodík, acetylén či acetonitril. Pri meraniach za teploty kvapalného dusíka bolo identifikovaných až 200 látok do molekulovej hmotnosti 500 g.mol-1. Aj pri meraniach za nízkej teploty boli dominantnými látkami acetonitril či diacetylene, no kyanovodík už tak dominantným nebol. Ďalej bolo v meraniach použité aj malé množstvo kyslíka, a za týchto podmienok boli významnými detegovanými látkami napr. formamid či acetón. Pri meraniach za laboratórnej aj nízkej teploty platilo, že so vzrastajúcou koncentráciou metánu vznikalo viac látok s vyššou molekulovou hmotnosťou a menej jednoduchých látok, ktoré sa pravdepodobne spotrebúvali na syntézu zložitejších látok. Rovnaká závislosť bola sledovaná aj pri narastajúcom výkone dodávanom do systému. Práca obsahuje aj merania pomocou iónovej mobilnej spektrometrie. Najvýznamnejším detegovaným plynom bol amoniak, ďalej bol detegovaný propan-2-ol, etanol a s najväčšou pravdepodobnosťou aj dietylamín. Poslednou sadou meraní boli merania pomocou FTIR, ktoré sú v zhode s výsledkami z PTR-TOF-MS. V spektre sú tiež vidieť intenzívne pásy prislúchajúce jak alifatickým uhľovodíkom (3050-2800 cm-1), tak aromatickým zlúčeninám (benzén na 1506 cm-1) a takisto aj pásy prislúchajúce dusíkom substituovaným uhľovodíkom (1350-1600 cm-1 a 3200-3400 cm-1). V spektre sú ďalej viditeľné píky HCN (713 cm-1) a C2H2 (729 cm-1), z ktorých boli zostrojené grafy závislostí na koncentrácii metánu.
The aim of this work is study of chemical processes in extraterrestrial atmospheres and the synthesis of organic compounds formed in electrical discharges in gaseous mixtures. Presented study focuses on the simulation of the atmosphere of Titan. The most common composition of the gaseous mixture was methane (1-4 sccm) in 200 sccm of nitrogen. Measurements with trace amounts of oxygen and carbon dioxide were also performed. In addition to the composition of the gas mixture, the experiments also varied the value of the electrical power delivered from 2 W - 12 W. The measurements were carried out at laboratory temperature but also at liquid nitrogen temperature, which made the experiment closer to the real conditions on Titan. Identification of the synthesized gaseous products in the reactor was carried out mainly by proton ionization mass spectrometry. Further measurements were using ion mobility spectrometry and Fourier transform infrared spectrometry. The discharge itself was characterised by optical emission spectrometry, confirming the presence of active nitrogen species and radicals arising from methane. In addition, the first negative and nitrogen second positive systems as well as the violet CN radical system were identified in the measured spectra. From the nitrogen second positive system, the rotational temperature was determined to be 2300 2400 K. The vibrational temperature was also determined from this system depending on the concentration of the gas mixture composition from 3100-3400 K. The vibrational temperature was calculated from the nitrogen first negative system, but it decreased slightly with methane concentration and increased with power in the interval from 3950-4350 K. The vibrational temperature obtained for the violet spectral CN system had similar dependence, with values ranging from 5900-7700 K. A number of aliphatic hydrocarbons, some aromatic hydrocarbons and also amino or cyano compounds were detected at laboratory temperature using a PTR-MS. The highest molecular weights at laboratory temperature were up to 150 g.mol-1 with hydrogen cyanide, acetylene or acetonitrile being the most abundant compounds. In measurements at liquid nitrogen temperature, nearly 200 substances up to a molecular weight of 500 g.mol-1 were identified. Even in low temperature measurements, acetonitrile or diacetylene were the dominant substances, but hydrogen cyanide was not so abundant as at ambient temperature. Small amount of oxygen was also used in the measurements and under these conditions, e.g. formamide or acetone were among the significant detected substances. In both laboratory and low-temperature measurements, it was confirmed that with increasing methane concentration, higher molecular weight substances were formed and lower number of simple substances were formed. The same dependence was observed with increasing power delivered to the system. The thesis also includes measurements by ion mobility spectrometry. The most important gas detected was ammonia, followed by propane-2-ol, ethanol and most likely diethylamine. The last measurements were obtained by FTIR. The basic spectrum shows bands belonging to aliphatic hydrocarbons (3050-2800 cm-1) and aromatic compounds (benzene at 1506 cm-1), nitrogen substituted hydrocarbons bands (1350-1600 cm-1 and 3200 3400 cm-1) were identified too. The spectrum further contains peaks of HCN (713cm-1) and C2H2 (729 cm-1) from which graphs of methane concentration dependence was obtained
The aim of this work is study of chemical processes in extraterrestrial atmospheres and the synthesis of organic compounds formed in electrical discharges in gaseous mixtures. Presented study focuses on the simulation of the atmosphere of Titan. The most common composition of the gaseous mixture was methane (1-4 sccm) in 200 sccm of nitrogen. Measurements with trace amounts of oxygen and carbon dioxide were also performed. In addition to the composition of the gas mixture, the experiments also varied the value of the electrical power delivered from 2 W - 12 W. The measurements were carried out at laboratory temperature but also at liquid nitrogen temperature, which made the experiment closer to the real conditions on Titan. Identification of the synthesized gaseous products in the reactor was carried out mainly by proton ionization mass spectrometry. Further measurements were using ion mobility spectrometry and Fourier transform infrared spectrometry. The discharge itself was characterised by optical emission spectrometry, confirming the presence of active nitrogen species and radicals arising from methane. In addition, the first negative and nitrogen second positive systems as well as the violet CN radical system were identified in the measured spectra. From the nitrogen second positive system, the rotational temperature was determined to be 2300 2400 K. The vibrational temperature was also determined from this system depending on the concentration of the gas mixture composition from 3100-3400 K. The vibrational temperature was calculated from the nitrogen first negative system, but it decreased slightly with methane concentration and increased with power in the interval from 3950-4350 K. The vibrational temperature obtained for the violet spectral CN system had similar dependence, with values ranging from 5900-7700 K. A number of aliphatic hydrocarbons, some aromatic hydrocarbons and also amino or cyano compounds were detected at laboratory temperature using a PTR-MS. The highest molecular weights at laboratory temperature were up to 150 g.mol-1 with hydrogen cyanide, acetylene or acetonitrile being the most abundant compounds. In measurements at liquid nitrogen temperature, nearly 200 substances up to a molecular weight of 500 g.mol-1 were identified. Even in low temperature measurements, acetonitrile or diacetylene were the dominant substances, but hydrogen cyanide was not so abundant as at ambient temperature. Small amount of oxygen was also used in the measurements and under these conditions, e.g. formamide or acetone were among the significant detected substances. In both laboratory and low-temperature measurements, it was confirmed that with increasing methane concentration, higher molecular weight substances were formed and lower number of simple substances were formed. The same dependence was observed with increasing power delivered to the system. The thesis also includes measurements by ion mobility spectrometry. The most important gas detected was ammonia, followed by propane-2-ol, ethanol and most likely diethylamine. The last measurements were obtained by FTIR. The basic spectrum shows bands belonging to aliphatic hydrocarbons (3050-2800 cm-1) and aromatic compounds (benzene at 1506 cm-1), nitrogen substituted hydrocarbons bands (1350-1600 cm-1 and 3200 3400 cm-1) were identified too. The spectrum further contains peaks of HCN (713cm-1) and C2H2 (729 cm-1) from which graphs of methane concentration dependence was obtained
Description
Keywords
Mesiac Titan, teórie o vzniku života, elektrické výboje v plynoch, optická emisná spektrometria, hmotnostná spektrometria protónovou ionizáciou, experimenty pri nízkych teplotách, infračervená spektroskopia s Fourierovou transformáciou, Titan moon, theories about origin of the life, electrical discharges in gases, optical emission spectrometry, proton transfer time of flight mass spectrometry, experiments at low temperature, Fourier transform infrared spectroscopy
Citation
CHUDJÁK, S. Štúdium chemických procesov v mimozemských atmosférach [online]. Brno: Vysoké učení technické v Brně. Fakulta chemická. 2022.
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Document version
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en
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Fyzikální chemie
Comittee
doc. Ing. Petr Dzik, Ph.D. (předseda)
prof. Ing. Květoslav Růžička, CSc. (člen)
doc. Ing. Pavel Čičmanec, Ph.D. (člen)
prof. Ing. Michal Čeppan, CSc. (člen)
prof. Ing. Martina Klučáková, Ph.D. (člen)
prof. RNDr. Štefan Matejčík, DrSc. (člen)
RNDr. Martin Ferus, Ph.D. (člen)
Date of acceptance
2022-09-30
Defence
Předseda komise představil doktoranda. Ing. Chudják má určité pracovní zkušenosti (2018-2021 Hartmann - Rico, 2021- dosud Baumüller Brno, s.r.o.), v letech 2018 - 2019 absolvoval odborně zaměřené kurzy a školení, 7 konferenčních příspěvků, 3 konferenční příspěvky a 3 příspěvky v journalech. Oponenti přečetli posudky, které byly kladné a doporučovaly práci k obhajobě. Posudky obsahovaly dotazy, na které doktorand uspokojivým způsobem odpověděl. Následně se rozproudila diskuze se členy komise.
Result of defence
práce byla úspěšně obhájena
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Standardní licenční smlouva - přístup k plnému textu bez omezení