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Deep Generated Methane in the Global Methane Budget

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Deep Generated Methane in the Global Methane Budget Deep generated methane in the global methane budget Elena D. Mukhina Doctoral Thesis 2018 KTH School of Industrial Engineering and Management Division of Heat and Power Technology SE-100 44 STOCKHOLM ii ISBN 978-91-7729-656-0 TRITA KRV Report 17/08 ISSN 1100-7990 ISRN KTH/KRV/17/08-SE © Elena Mukhina Stockholm 2018 [email protected] Academic thesis, which with the aproval of Royal Institute of Technology (KTH), will be presented in fulfillment of the requirements for the Degree of Doctor of Philisophy, Public defence is in Room Kollegiesalen, at KTH Royal Institute of Technology, Stockholm, at 13:00, on the 14th of March 2018. iii Abstract Methane is a significant part of the global carbon cycle. The distribution of methane above and below the Earth’s surface suggests that atmospheric methane might be related to methane originating from the deep mantle. The purpose of the present study is to identify this relationship between methane emissions to the atmosphere and methane, which can be abiogenically generated within the Earth’s interior. Methane hydrates within the Earth’s surface sediments might be among the possible hosts of migrated deep methane. In this thesis, experimental work is presented, which aimed to reveal the depth at which methane and other hydrocarbons in the upper mantle are abiogenically generated, considering pT and redox conditions of the surrounding environment. High-pressure, high-temperature experiments were conducted using a large reactive volume device with a toroid-type chamber in specially prepared sample containers. The present study evaluates the formation of methane and other hydrocarbons at temperatures higher than 300 °C at pressures of 2.5-6.5 GPa despite the redox conditions of the surroundings. These conditions correspond to a depth below 70 km on the surface of a cold subducting slab. The proposed hypothesis claims that the deep-mantle-generated methane can contribute to the formation of methane hydrates and accumulation of free gas below hydrates. Keywords: methane hydrates, methane emissions, deep abiogenic origin of hydrocarbons, redox, high pressure, high temperature, toroid-type chamber, chromatography, subduction zone, upper mantle, mid-ocean ridge. iv Preface The present publication is devoted to revealing the connection between mantle-generated methane and methane emissions from the Earth’s surface. This thesis is divided into four chapters. The introduction provides a brief overview of the pillars of the present thesis, which are methane emissions on Earth, methane hydrates and their contribution to methane emissions, and the concept of the deep mantle origin of hydrocarbons. The objectives and research questions of the present study are also included in Chapter 1. Chapter 2 explains the choice of the methods used in the work and describes in detail the experimental procedure that was performed, including a newly developed improvement of the sample-carrying technique. Chapter 3 focuses on the experimental investigation of redox and pT conditions that are favorable for deep mantle methane formation. It describes how surrounding influences the formed hydrocarbon systems. All experimental results are described in this chapter with the implication of the geological environment, predicting the depth of the studied processes. Chapter 4 introduces a new hypothesis of the deep-mantle-originated methane contribution to the formation of methane hydrates within the Earth’s surface sediments. v Acknowledgements First, I would like to thank my main supervisor, Vladimir Kutcherov, who gave me the opportunity to study at KTH, who has arranged my studying and always managed all problems on our way to my defense. Thanks to him I was able to learn everything I know, including how to work as a part of a team or how to be self-sustained. Thanks to Vladimir I have significantly grown up as a scientist and as a person. I am grateful to all my project colleagues, Anton, Alexandr and Daniil, who brought a lot to experimental procedures and discussions. I thank the physics department at Gubkin University, Moscow, Russia, where all experiments were carried out. Many thanks to my colleagues from BGI Bayerisches Geoinstitut, Bayreuth, Germany, and especially to Leonid Dubrovinsky, for priceless knowledge I have obtained during my traineeship in 2015 and scientific and social contacts. I would like to express my sincere gratitude to my family and friends, who supported me during my years of studying. Special thanks to my dearest friend Leyla, who has supported and inspired me. Special thanks to my mother for relentless believing in me, who cared about me more than anyone. Finally, I would like to express my heartfelt gratitude to Ksenia for all the encouragement she gave me and for being there for me every day through the hardest period of my studying. Financial support was granted by Russian Global Education Program (GEP) and Sloan Foundation through the Deep Carbon Observatory. Stockholm, January 2018 Elena D. Mukhina vi List of appended papers Paper A E. Mukhina, A. Kolesnikov & V. Kutcherov, The lower pT limit of deep hydrocarbon synthesis by CaCO3 aqueous reduction, Scientific Reports, 7 (5749), 2017, doi:10.1038/s41598-017-06155-6 Paper B E.D. Mukhina, D.A. Kudryavtsev, A.Yu. Kolesnikov, A.Yu. Serovaisky, V.G. Kutcherov, The influence of a sample container material on high pressure formation of hydrocarbons, Materials Research Express Paper C E. Mukhina, A. Kolesnikov, D. Kudryavtsev, L. Dubrovinsky, V. Kutcherov, Deep genesis of hydrocarbons under oxidized conditions Paper D E.D. Mukhina, A.Yu. Kolesnikov, A.Yu. Serovaiskii, V.G. Kutcherov, Experimental Modelling of Hydrocarbon Migration Processes, Journal of Physics: Conf. Series, 950 (042040), 2017, doi:10.1088/1742-6596/950/4/042040 Related publications V.G. Kutcherov, A.Yu. Kolesnikov, E.D. Mukhina, A.Yu. Serovaisky, Teaching aid “High-pressure high-temperature experimental studies”, Gubkin Russian State University, 2016; D. Kudryavtsev, A. Serovaiskii, E. Mukhina, A. Kolesnikov, B. Gasharova, V. Kutcherov, L. S. Dubrovinsky, Raman and IR Spectroscopy Studies on Propane at Pressures of Up to 40 GPa, The Journal of Physical Chemistry A, 121 (32), 2017, doi: 10.1021/acs.jpca.7b05492 A.Yu. Serovaiskii, A.Yu. Kolesnikov, E.D. Mukhina, V.G. Kutcherov, The photochemical reaction of hydrocarbons under extreme thermobaric conditions, Journal of Physics: Conf. Series, 950 (042056), 2017, doi: 10.1088/1742- 6596/950/4/042056 vii Authors’ contributions The objectives of the project were developed by E. Mukhina under the guidance of the main supervisor associate professor V. Kutcherov. E. Mukhina performed all experiments and data analyses described in the present thesis. E. Mukhina wrote all texts for all appended papers, and as the corresponding author for all papers, prepared and revised them for publication after co- authors’ advises and comments. viii Definition of critical terms and nomenclature Methane hydrate – a solid clathrate compound composed of methane molecules, trapped within water dodecahedron crystals. The appearance is similar to regular water ice. Subduction – occurs along a tectonic boundary, where one tectonic plate sinks under an opposite one into the Earth’s mantle. Part of the plate sunk into the mantle is a subducting slab. Mid-ocean ridge – a ridge of seafloor mountains, created by spreading of tectonic plates. Redox conditions – conditions, specified by the tendency of the environment to be oxidized or reduced. pT parameters, thermobaric conditions – pressure (GPa) and temperature (°C) List of abbreviations DAC – diamond anvil cell LRV – large reactive volume FID – flame ionization detector XRD – X-ray diffrection HP – hyperfine parameters CS – central shift QS – quadrupole splitting MF – magnetic field C – carbon List of notations V – volume m – mass ρ – density M – molar mass n – amount of substance P – pressure T – temperature 2θ – diffraction angle ix Contest Abstract ......................................................................................................................... iii Preface .......................................................................................................................... iv Acknowledgements .........................................................................................................v List of appended papers ............................................................................................... vi Authors’ contributions ................................................................................................. vii Definition of critical terms and nomenclature .......................................................... viii Contest .......................................................................................................................... ix Chapter 1. Introduction ................................................................................................ 1 1.1. Anthropogenic and natural methane emissions ............................................... 1 1.2. Methane hydrates as natural methane emitters .............................................. 6 1.3. The abiogenic origin of hydrocarbons. Experimental works .......................... 12 1.4. The main objective, research questions and structure of the dissertation .... 15 Chapter 2. Methodology of the experimental study on high-pressure hydrocarbon formation. ..................................................................................................................... 17 2.1.
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