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Using secondary minerals and hydrochemistry to trace geochemical processes in the deep subsurface. Henrik Drake Linnaeus University, Sweden

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using secondary minerals and hydrochemistry to trace geochemical processes in the deep subsurface

Using secondary minerals and hydrochemistry to trace geochemical processes in the deep subsurface

Henrik Drake

Linnaeus University, Sweden

Co-workers: LnU/SKB: Mats Åström, Olga Maskenskaya, Changxun Yu, Frederic Mathurin, Tobias Berger, Linda Alakangas, Birgitta Kalinowski, Ignasi Puigdomenech, Elsewhere: Eva-Lena Tullborg, Johan Hogmalm, Martin Whitehouse, Christine Heim, Magnus Ivarsson, Bill Wallin, Curt Broman, Thomas Zack, etc etc

billion years of history
Billion years of history

Present Groundwaters

Deep Saline Glacial Marine Meteoric

>~500ka 14ka 4-8ka present recharge

Start of mix with brine at 10 Ma

Presently active bacteria

SRB, IRB etc

?

Past activity?

Salinity?

Redox?

Hydrothermal history

Possible Quaternary

slide3
Methodology

Microscope/SEM

Fluid inclusions

Trace elements

Biomarkers

Geochronology

Fracture orientations

Isotopes

Drake and Tullborg, 2009, AG

Drake et al., in press, AG

Mathurin et al., ES&T (2012)

Drake et al., 2012, GCA

Maskenskaya et al.,

submitted

hydrothermal
Hydrothermal

References:

Drake et al. 2009 Lithos,

Drake and Tullborg, 2009 Appl. Geochem

Drake et al. 2012, GCA, 2013, GCA

Maskenskaya et al., submitted x 2

hydrothermal1
Hydrothermal

Berger et al., 2013

Drake et al., 2013 GCA

Laaksoharju et al., 2009

Mathurin et al., in press GCA

low temperature minerals
Low temperature minerals
  • Recent past conditions (0-10 Ma = minerals, and groundwater 0-0.5 Ma), 0-1000 m
  • Near-surface redox front
  • Fresh/saline interface and
  • Trace element variation/Trace element uptake into calcite
  • Activity of bacteria
    • Sulphate reducers
    • Methanogens
    • Methane oxidation
    • (Iron-reducers)
  • Pre-drilling, undisturbed conditions (minerals)
redox front
Redox front

Can be detected examining redox sensitive minerals and elements

slide8

CeIII CeIV

Oxides

Drake et al., in prep

Yu et al., in prep

Drake et al., 2009, Appl.Geochem

Drake et al., 2009 Appl.Geochem

slide10

TRACE METAL INCORPORATION (CALCITE)

Drake et al., (2012, GCA)

Maskenskaya et al., submitted

Also fracture-zone scale variability

Drake et al., (2013, Appl. Geochem.)

slide12

This study

Drake et al., 2013, GCA

Samples:

Groundwater

(δ34S, SO4, DOC, HCO3)

Pyrite (δ34S)

0 - >900 m depth

Mathurin et al., (2012)

pyrite
Pyrite
  • huge variations across individual crystals (-32 to +73‰)
  • extreme minimum (-50‰) and
  • maximum (+91‰) values.
  • =>141‰ range!
  • SRB activity at all depths analysed, 0-900 m
  • intra-crystal δ34S pattern
  • Increase with growth

Drake et al., 2013, GCA

34 s rim 34 s centre vs so 4
δ34Srim- δ34Scentre vs.SO4

Drake et al., 2013, GCA

ongoing future studies 1 traces of methane oxidation methanogenesis drake et al in prep
ONGOING/FUTURE STUDIES:1. TRACES OF METHANE-OXIDATION/METHANOGENESISDrake et al., in prep
slide16

Calcite (δ13C, δ18O)

0 - >900 m depth

Drake et al.,in press

Appl. Geochem

SIMS10 µm in situ analysis

+ToF-SIMS/GC-MS

slide17

Methanogenesis

(up to c. +5 per mil)

Small organic influence

Min: -125‰

Influence of organic C, e.g. from plants

Anaerobic oxidation

of methane

(biomarkers are SRB-

specific of high AOM-specificity, ToF-SIMS+GC/MS data)

Drake et al., in prep

slide18

Methanogenesis

(up to c. +5 per mil)

Min: -125‰

Drake et al., in prep

similar study from forsmark
Similar study from Forsmark

Methanogenesis

(to +12 per mil)

Anaerobic oxidation

of methane

stable isotope variation and trace element uptake in recent 17y precipitates at sp
Stable isotope variation and trace element uptakein recent, <17y, precipitates at Äspö
  • Micro-variation of sulphur isotopes in pyrite
  • Trace element uptake in calcite
slide21

PRECIPITATES ON BOREHOLE EQUIPMENT AT ÄSPÖ (-450 m)

Mathurin et al., ES&T (2012)

Drake et al., in prep

slide23

MICRO-SCALE S-ISOTOPE VARIATION

δ34Ssulphate +18 to +28‰

δ34Ssulphide -29 to -1‰

Iron isotopes to be added,

First SIMS results of fracture-

coating pyrite δ56Fe -0.9 to +2.8‰

Drake et al., in review

slide24

TRACE METAL INCORPORATION INTO CALCITE

+Ba, LREEs

(+Y, V)

(not shown)

Drake et al., in prep

finally this area has
Finally,this area has
  • Most depleted δ13Ccalcite reported (-125‰)
  • Largest δ13Ccalcite range within a single crystal (109‰)
  • Largest range of δ13Ccalcite from single location (129‰)
  • Largest δ34Spyrite range from single location (141‰; Drake et al., 2013, GCA)
  • Thank you!

δ34S

δ13C

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