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The Organic Chemistry of Volcanic Gases at Vulcano (Aeolian Islands, Italy)

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The Organic Chemistry of Volcanic Gases at Vulcano (Aeolian Islands, Italy) Diss. ETH No. 14706 The Organic Chemistry of Volcanic Gases at Vulcano (Aeolian Islands, Italy) A dissertation submitted to the SWISS FEDERAL INSTITUTE OF TECHNOLOGY ZÜRICH for the degree of Doctor of Natural Sciences presented by Florian Maximilian Schwandner Dipl. Geol-Paläontol., Freie Universität Berlin born August 13th, 1970 citizen of the Federal Republic of Germany accepted on the recommendation of Prof. Dr. T.M. Seward Inst. of Mineralogy and Petrography, ETH Zürich examiner Prof. Dr. V.J. Dietrich Inst. of Mineralogy and Petrography, ETH Zürich co-examiner Dr. A. P. Gize Dept. of Earth Sciences, University of Manchester (UK) co-examiner 2002 To my family i Preface Finally the printed “Pflichtexemplar” (mandatory copy) is done and printed, and life after the PhD can continue. In addition to the acknowledgements at the end of this thesis, a few remarks seem appropriate at this point. It has been a great pleasure and experience to conduct this work, with the professional, financial and personal support of Terry Seward, Volker “Wumme” Dietrich, Andy Gize, Jenny Cox, a variety of other colleagues as well as my family and friends. Christoph Wahrenberger preceeded me on the research topic and Alex Teague will continue on after me but I am sure there will be many more scientists “jumping on the train” in the nearest future. There has been, still is and probably always will be great resistance to innovative ideas and approaches in science, especially by people who are so unfortunate to heavily depend on funding raised by and for mainstream “politically correct” research, or catastrophism. The idea to find permanent natural sources of natural halocarbons from volcanoes is not new but despite ist scientific foundation is still facing resistance. If a theory persists and dominates for a long time, then it eventually becomes a “fact” in many peoples eyes. This leads to publications starting with the phrase “It is well known that...”. To put the topic of this thesis in that context: many papers about halocarbons and ozone depletion for example contain the phrase “halocarbons are solely of anthropogenic origin” (or similar formulations). In this PhD research, I had to learn that a strong scientific lobby exists that carries out research on anthropoghenic releases. To question one of their often stated basic assumptions (i.e. the phrase “halocarbons are solely of anthropogenic origin”) is in some ways threatening to “take the butter off their bread”, as an old German saying goes. The peer-reviewing of project funding proposals is therefore possibly sometimes hindering innovative ideas. However, an increasing number of research groups is since the nineties indeed focusing on natural sources of halocarbons. It reminds me of a quote by Rabindranath Tagore (1861-1941; 1913 Nobel Laureate in Literature), “The false can never grow into truth by growing in power”("Stray Birds", 1916). The answer therefore has to be, to provide rigorous unbiased scientific evidence. F.M. Schwandner, Zürich, August 28th, 2002 Preface ii Table of contents Preface i Abstract iv Zusammenfassung (German abstract) vi Chapter I Introduction 1 Chapter II Halocarbons and other organic compounds in volcanic gases from Vulcano (Aeolian Islands, Italy) 7 Abstract 8 1. Introduction 9 2. Previous work 11 3. Volcanic impacts to the atmosphere 14 3.1. Global warming 14 3.2. Ozone depletion 17 4. Experimental 24 4.1. Sampling and preparative work 24 4.2. Analysis 26 4.3. Data treatment 27 4.4. Contamination, sample loss, degradation and blanks 30 5. Results 35 5.1. Hydrocarbons 35 5.2. Oxygenated compounds 42 5.3. Heteroatomic compounds excluding halocarbons and oxygenated hydrocarbons 43 5.4. Halocarbons 45 5.5. Other compounds 51 6. Flux estimates of volcanic halocarbon emissions 52 6.1. Total carbon fluxes and carbon recycling 52 6.2. Total halogen fluxes 52 6.3. Trace gas correlations 53 6.4. Single compound static flux estimate 56 6.5. Dynamic volcanogenic trace gas flux model 57 7. Discussion 63 7.1. Origin of source material 63 7.2. Variation with type of magmatic activity and/or tectonic setting 64 7.3. Processes of formation 65 8. Implications for further research and outlook 77 8.1. Atmospheric chemistry 77 8.2. Volcanic gas studies, exploration and volcanic surveillance 81 8.3. Metal transport in hydrothermal fluids 82 8.4. Origin of life and abiogenic hydrocarbons 84 9.Summary 85 Table of Contents iii Chapter III Diffusive emission of organic trace gases from the flanks and crater of a quiescent active volcano (Vulcano, Aeolian Islands, Italy) 89 Abstract 90 1. Introduction 91 2. Experimental 93 2.1. Sample collection 93 2.2. Analytical methods 96 3. Results 99 3.1. Site parameters and CO2-flux 99 3.2. Chemical parameters 102 4. Summary and discussion 116 4.1. Vegetation effects and adsorption on soil particles 116 4.2. The crater region 118 4.3. Pyrolysis 119 4.4. Abiogenic formation 120 Chapter IV Conclusions 123 References 127 Appendix A1. A historic overview of organic chemical volcanic gas studies A1.1 A2. Additional GC-MS method information A2.1 A3. Chromatograms & mass spectra A3.1 Acknowledgements Curriculum vitae Table of Contents iv Abstract In order to assess the source strength, composition and formation of trace organic constituents in volcanic gas emissions, we collected a total of 48 samples of sorbent-trapped volcanic gases, sublimates, condensates from active vents of the La Fossa crater on the island of Vulcano (Aeolian Islands, Italy) as well as ambient and industrial air, during three sampling campaigns in the years 1999, 2000 and 2001. Previously, trace organic gas analyses from volcanic sources have been limited by analytical problems such as the strong sulfur, halogen acid and water matrix that is deleterious to sensitive trace organic analysis by GC-MS. We developed a novel analytical and sampling approach that allows reliable, sensitive and quantitative analysis by Short-Path Thermal Desorption-Solid Phase Microextraction- Cryotrapping-Gas Chromatography/Mass Spectrometry (SPTD-SPME-CF-GC-MS. In a total of 158 GC-MS analyses we detected and selectively quantified well over 100 compounds in each sample. We found alkanes, alkenes, arenes, phenols, aldehydes, carboxylic acids, esters, ketones, nitriles, furans, PAH's and their halogenated, methylated and sulfonated derivatives, as well as various heterocyclic compounds including thiophenes. Most compounds are present at concentrations well above laboratory, ambient air, adsorbent and field blank levels. For some analytes (e.g., CFC-11, CH2Cl2, CH3Br), concentrations are up to several orders of magnitude greater than even mid-latitudinal industrial urban air maxima. Air or laboratory contamination is negligible or absent on the basis of inert gas and noble gas isotopic measurements. The organic compounds are interpreted as the product of inorganic, abiogenic gas-phase radical reactions. On the basis of isomer abundances, n-alkane distributions and the substitution pattern the compounds are considered to have been formed by high temperature (e.g., 900 °C) alkyl free radical reactions and halide electrophilic substitution on arenes, alkanes and alkenes. Model global volcanic halocarbon fluxes from our own and published compositional data on a number of halocarbons have been obtained by scaling to published volcanic CO2 fluxes. This -9 -1 -4 -1 yields global halocarbon fluxes in the range from 1.0x 10 Tg y (CClF3) to 1.2 x 10 Tg y (CH3Cl). Methyl bromide (CH3Br) and methyl iodide (CH3I) are estimated to have a volcanic model source strength of up to 1.3 x 10-6 Tg y-1, however, it is noted that other brominated Abstract v compounds were identified. The significance of organic emissions from quiescent volcanic degassing as opposed to explosive eruptions to stratospheric chemistry is that the negligible aqueous solubility of most emitted organic compounds does not lead to a quantitative tropospheric washout effect as postulated for explosive volcanic HCl and HF emissions. Simple modeling suggests that episodic, catastrophically large, explosive events such as flood basalt eruptions do not impact the short-term ozone chemistry to the same magnitude as today’s anthropogenic emissions but may modify the natural atmospheric reactive balance over much longer (geological) time spans. In addition, the apparent abiogenic organic chemistry of volcanic gases may give insights into the possible hydrothermal origin of early life on Earth, as indicated by the presence of simple amino acids, nitriles, and alkanoic acids. In order to clarify the source of these compounds we have sampled soil gas emissions of organic compounds and determined CO2 fluxes along a profile spanning from the vegetated base of the active La Fossa cone (Vulcano Island, Italy) over the unvegetated volcanic flank, the crater rim and base, into fumarolic areas. The results indicate that a) the majority of volatile organic compounds in the soil gas show significant increases in concentration towards the crater and fumaroles, b) emissions of the 2 halocarbon CFC-11 (CCl3F) correlate well with soil CO2 fluxes measured on site (R =0.91 ±0.02) and both increase towards the crater and fumaroles, and c) diffusive emissions therefore contribute significantly to the volcanic halocarbon source strength. Other ozone depleting substances were found in concentrations significantly above those found in field and system blanks, including CH3Br, CH3Cl, CH3I, C2H5Br, and chlorinated benzenes. Abundances range from upper pptv to ppmv (e.g. CFC-11: max. 1200 pptv diffusive, 3700 pptv fumarolic/dry gas, dry air: 268 pptv). On the basis of these results, the natural volcanic source strength of halocarbon emissions to the atmosphere requires re-evaluation and correction to higher values. Abstract vi Zusammenfassung Drei Beprobungskampagnen wurden in den Jahren 1999, 2000 und 2001 auf dem aktiven La Fossa Vulkan auf der Insel Vulkano (Aeolische inseln, Italien) durchgeführt, um die Quellstärken, Zusammensetzung und Formationsprozesse organischer Spurengase in vulkanischen Exhalationen zu charakterisieren.
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