C- and N-Bearing Species in Reduced Fluids in the Simplified C-O-H-N System and in Natural Pelite at Upper Mantle P-T Conditions

C- and N-Bearing Species in Reduced Fluids in the Simplified C-O-H-N System and in Natural Pelite at Upper Mantle P-T Conditions Full article

Journal

Minerals
ISSN: 2075-163X

Output data

Year: 2019, Volume: 9, Number: 11, Article number : 712, Pages count : DOI: 10.3390/min9110712

Tags

mantle; subduction; pelite; fluid; hydrocarbons; methanimine; deep carbon cycle; deep nitrogen cycle

Authors

Sokol Ivan ¹ , Sokol Alexander ^1,2 , Bul'bak Taras ¹ , Nefyodov Andrey ³ , Zaikin Pavel ³ , Tomilenko Anatoly ¹

Affiliations

1	V.S. Sobolev Institute of Geology and Mineralogy, Siberian Branch of the Russian Academy of Sciences (IGM SB RAS), 3, Koptyug ave., 630090 Novosibirsk, Russia
2	Novosibirsk State University, 2, Pirogov str., 630090 Novosibirsk, Russia
3	N.N. Vorozhtsov Novosibirsk Institute of Organic Chemistry, Siberian Branch of the Russian Academy of Sciences, 9, Lavrentiev ave., 630090 Novosibirsk, Russia

C- and N-bearing species in reduced fluids weree studied experimentally in C-O-H-N and muscovite-C-O-H-N systems and in natural carbonate-bearing samples at mantle P-T parameters. The experiments reproduced three types of reactions leading to formation of hydrocarbons (HCs) at 3.8-7.8 GPa and 800-1400 degrees C and at hydrogen fugacity (fH(2)) buffered by the Fe-FeO (IW) + H2O or Mo-MoO2 (MMO) + H2O equilibria: (i) Thermal destruction of organic matter during its subduction into the mantle (with an example of docosane), (ii) hydrogenation of graphite upon interaction with H-2-enriched fluids, and (iii) hydrogenation of carbonates and products of their reduction in metamorphic clayey rocks. The obtained quenched fluids analyzed after the runs by gas chromatography-mass spectrometry (GC-MS) and electronic ionization mass-spectrometry (HR-MS) contain CH4 and C2H6 as main carbon species. The concentrations of C-2-C-4 alkanes in the fluids increase as the pressure and temperature increase from 3.8 to 7.8 GPa and from 800 to 1400 degrees C, respectively. The fluid equilibrated with the muscovite-garnet-omphacite-kyanite-rutile +/- coesite assemblage consists of 50-80 rel.% H2O and 15-40 rel.% alkanes (C-1 > C-2 > C-3 > C-4). Main N-bearing species are ammonia (NH3) in the C-O-H-N and muscovite-C-O-H-N systems or methanimine (CH3N) in the fluid derived from the samples of natural pelitic rocks. Nitrogen comes either from air or melamine (C3H6N6) in model systems or from NH4+ in the runs with natural samples. The formula CH3N in the quenched fluid of the C-O-H-N system is confirmed by HR-MS. The impossibility of CH3N incorporation into K-bearing silicates because of a big CH3NH+ cation may limit the solubility of N in silicates at low fO(2) and hence may substantially influence the mantle cycle of nitrogen. Thus, subduction of slabs containing carbonates, organic matter, and N-bearing minerals into strongly reduced mantle may induce the formation of fluids enriched in H2O, light alkanes, NH3, and CH3N. The presence of these species must be critical for the deep cycles of carbon, nitrogen, and hydrogen.

Sokol I. , Sokol A. , Bul'bak T. , Nefyodov A. , Zaikin P. , Tomilenko A.
C- and N-Bearing Species in Reduced Fluids in the Simplified C-O-H-N System and in Natural Pelite at Upper Mantle P-T Conditions

Minerals. 2019. V.9. N11. 712 . DOI: 10.3390/min9110712 WOS Scopus РИНЦ РИНЦ

Full text from publisher

Published online:

Nov 18, 2019

Web of science	WOS:000502267100065
Scopus	2-s2.0-85075504397
Elibrary	41409386 , 43207430
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