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Oil and Gas E&P --------------------------------------------------------------------- Domestic Gas Supply -----------------------------------LNG Distribution --------------- New Technologies
JAPEX operates 10 oil & gas production fields in Japan including offshore platform, underground gas storage using natural reservoir, mini-LNG, and world’s only LNG transport by train, to ensure stable gas delivery to our customers.
Three-dimensional reactive transport simulation of the CCS demonstration project
in Tomakomai, Hokkaido, Japan
GastechMakuhari, Chiba
4 April 2017
Kohei Akaku1, Fumiaki Okumura1, Susumu Okubo1, Yusuke Wasaki1, Junji Yamamoto1, Hajime Yamamoto2, Yusuke Hiratsuka2, Takayasu Honda3 and Takahiro Nakajima4
1Japan Petroleum Exploration Co., Ltd. (JAPEX)2Taisei Corporation3Japan CCS Co., Ltd. (JCCS)4Research Institute of Innovative Technology for the Earth (RITE)
2
• CO2 trapping mechanism• Geochemical reaction model for Tomakomai project• One-dimensional reactive transport simulation• Three-dimentional reactive transport simulation• Conclusions
TOUGHREACT version 2.0 (LBNL) revised in RITEThermoddem database (BRGM)
3
Outline
Reservoirs and cap rocks of the Tomakomai CCS demonstration Project 4
Reservoir
Cap rock
※Aspect Ratio=1:1
Injection Well for
Moebetsu Fm.
Injection Well for
Takinoue Fm.
(projected)
Cap rock
Reservoir
Landward(North) Seaward(South)
T1 Member of Takinoue Fm. (Volcanic Rocks)
Fureoi Fm. (Mudstone)
Quaternary sediments
Moebetsu Fm. (Mudstone)
Takinoue Fm. (Mudstone)
Nina Fm. (Mudstone)
Moebetsu Fm. (Sandstone)
Mukawa Fm. (Sandstone, Mudstone, etc.)
Biratori-Karumai Fm. (Mudstone)
Depth
in
mete
rs (
bM
SL)
(TD 5,800m)
(TD 3,650m)
Observation Well
for Moebetsu Fm.
Copyright 2017 Japan CCS Co., Ltd.
CO2 storage mechanisms in geological formations
http://www.co2captureproject.org/co2_trapping.html
IPCC (2005)
• The effectiveness of geological storage depends on a combination of physical and geochemical trapping mechanisms.
Structural and stratigraphic trapping is primarily important.
Residual trapping due to capillary forces and solubility trapping in water are highly important, too.
The forth mechanism, mineral trapping, is believed to be slow, potentially taking a thousand years or longer.
• What is going on in the Moebetsu Formation?
5
Analysis of water and its thermodynamic reconstruction
• Why do we need thermodynamic reconstruction? Ideally, formation water should be in
equilibrium with diagenetic minerals. But… Concentrations of minor components (Al3+,
HS-) are not usually obtained through the water analysis.
Degassing and mineral precipitation before water sampling.
• On the other hand… Thermodynamic database for solubility of
minerals and aqueous ion properties is not always perfect.
Native minerals are too complex structures and compositions.
The reconstruction is a validation step of the following reactive transport simulation.
• A good result with Thermoddem (BRGM, 2014).
6
Analyzed composition
Tomakomai well OB-2
Thermodynamically
reconstructed water
Temperature (°C) 44
pH 8.34 7.11
mg/kg
Cl- 1942 1907
SO42- 9.16 9.20
HCO3- 731 608
HS- not analyzed 0.000111
SiO2(aq) 74.4 165
Al3+ not detected 0.0000401
Ca2+ 78.5 39.1
Mg2+ 13.7 6.43
Fe2+ 0.30 0.85
K+ 26.6 26.7
Na+ 1365 1371
NH4+ 2.7 2.71
Remarks
The pH measured at
atmospheric pressure
and room temperature.
Equilibrium with pyrite,
amorphous silica, Na-
clinoptilorite, kaolinite,
siderite, magnesite, calcite,
Fe-Na-saponite.
Mineral saturation indices (log Q/K) of the reconstructed water
• Reconstructed water is under-saturated with the detrital minerals (plagioclase, glauconite, biotite, serpentinite, pyroxene and amphibole).
• The formation water does not possibly react well with these minerals.
• Over-saturated with quartz, K-feldspar and chlorite is probably due to kinetic barrier at low temperature.
7
Minerals Compositions
Saturation
index
in water
logQ/K
Rock forming minerals
quartz SiO2 0.96
plagioclase (albite/anorthite) Na0.5Ca0.5Al1.5Si2.5O8 -2.37
K-feldspar KAlSi3O8 1.62
calcite CaCO3 0.00
saponite(FeNa) Na0.34Mg2FeAl0.34Si3.66O10(OH)2 0.00
kaolinite Al2(Si2O5)(OH)4 0.00
chlorite (clinochlore/daphnite) Mg2.5Fe2.5Al2Si3O10(OH)8 2.15
glauconite (K0.75Mg0.25Fe1.5Al0.25)(Al0.25Si3.75)O10(OH)2 -1.44
serpentinite Mg3Si2O5(OH)4 -5.17
biotite (siderophyllite/eastonite) KFeMgAl3Si2O10(OH)2 -5.18
clinoptilolite(Na) Na1.1(Si4.9Al1.1)O12:3.5H2O 0.00
pyrite FeS2 0.00
pyroxene (diopside/hedenbergite) CaMg0.8Fe0.2Si2O6 -3.87
amphibole (tremolite/actinolite) Ca2(Mg3Fe2)Si8O22(OH)2 -5.93
Secondary minerals
amorphous silica SiO2 0.00
siderite FeCO3 0.00
magnesite MgCO3 0.00
dawsonite NaAlCO3(OH)2 -2.08
dolomite (ordered) CaMg(CO3)2 -0.26
Kinetic parameters
• Kinetic rate constants and activation energies for dissolution of minerals are from literature (e.g. Palandri and Kharaka, 2004).
• Reactive surface area of minerals is the most uncertain parameter. The standard values for sandstone grain size are quoted from Xu et al. (2011).
• Based on the batch reaction simulation without CO2 injection, we decided…
Reduce the reactive surface areas for the under-saturated detrital minerals by 3-5 orders of magnitude, except for glauconite
Precipitation of the over-saturated minerals was suppressed
• Nearly stable water composition through 10,000 years. Reasonable model!
K
QkAr
m
mmmm 1
15.29811
exp25
TRE
kka
m
8
MineralsMineral
composition
Kinetic rate
constants
Activation
Energy
Reactive
surface area
vol%log(k) 25°C
(mol/m2/s)
Ea
(kJ/mol)
A
(cm2/g)
Rock forming minerals
quartz 36.11 -13.40 90.9 9.1
plagioclase (albite/anorthite) 25.84 -10.91 45.2 9.1.E-04
K-feldspar 2.36 -12.41 38.0 9.1
calcite 0.10 -5.81 23.5 9.1
saponite(FeNa) 0.09 -14.41 48.0 108.7
kaolinite 6.34 -13.18 22.2 108.7
chlorite (clinochlore/daphnite) 0.95 -12.52 88.0 9.1
glauconite 12.42 -9.10 85.0 9.1
serpentinite 2.24 -12.00 73.5 108.7E-3
biotite (siderophyllite/eastonite) 9.51 -12.55 22.0 108.7E-3
clinoptilolite(Na) 2.74 -12.63 58.0 9.1
pyrite 0.27 -10.40 62.7 12.9
pyroxene (diopside/hedenbergite) 0.33 -11.11 40.6 9.1.E-04
amphibole (tremolite/actinolite) 0.69 -10.60 94.4 9.1.E-05
Secondary minerals
amorphous silica -9.42 49.8 9.1
siderite -8.90 62.8 9.1
magnesite -9.34 23.5 9.1
dawsonite -7.00 62.8 9.1
dolomite (ordered) -8.60 95.3 9.1
Results of one-dimensional (1D) simulations
0%
10%
20%
30%
40%
50%
60%
70%
80%
90%
100%
1 10 100 1000 10000
CO
2tr
app
ed
(%)
Time since injection starts (years)
溶存CO2
鉱物CO2
超臨界CO2
-2.0E+9
-1.5E+9
-1.0E+9
-5.0E+8
0.0E+0
5.0E+8
1.0E+9
1.5E+9
2.0E+9
1 10 100 1000 10000
Changes in m
inera
l abundance
(mo
l)
Time since injection starts (years)
石英
非晶質シリカ
斜長石
カリ長石
方解石
シデライト
マグネサイト
ドーソナイト
ドロマイト
FeCa-サポ
ナイトカオリナイト
緑泥石
海緑石
蛇紋石
黒雲母
黄鉄鉱
Na-斜プチロ
ル沸石
0%
10%
20%
30%
40%
50%
60%
70%
80%
90%
100%
1 10 100 1000 10000
CO
2tr
app
ed
(%)
Time since injection starts (years)
溶存CO2
鉱物CO2
超臨界CO2
-2.0E+9
-1.5E+9
-1.0E+9
-5.0E+8
0.0E+0
5.0E+8
1.0E+9
1.5E+9
2.0E+9
1 10 100 1000 10000
Changes in m
inera
l abundance
(mol)
Time since injection starts (years)
石英
非晶質シリカ
斜長石
カリ長石
方解石
シデライト
マグネサイト
ドーソナイト
ドロマイト
FeCa-サ
ポナイトカオリナイト
緑泥石
海緑石
蛇紋石
黒雲母
黄鉄鉱
Na-斜プチ
ロル沸石
glauconite
amorph silicasiderite
calcite
kaolinite
magnesite
Moebetsu, inj-MN1(1D)
pyrite
aqueous
super-critical mineral
aqueous
super-critical
mineral
glauconite
amorph silica
siderite
calcite
kaolinite
magnesite
precipitation
dissolution
precipitation
dissolution
chloritechlorite
Moebetsu, inj-MN3(1D)
Reactive surface area of glauconite was reduced by 4 orders of magnitude for “inj-MN3”.
• 45 m thickness• 44°C• Φ=28.1%• k=233 mD• 50,000 tons/year for 3 years• TOUGHREACT
• Prominent reactions Dissolution of glauconite Precipitation of amorphous
silica and kaolinite CO2 trapped by precipitation
of siderite and magnesite
• Mineral trapping of CO2 depends on the reactive surface area of glauconite. 85% mineral trapped in “inj-
MN1” model at 1,000 years 20% in “inj-MN3” model at
10,000 years
9
Results of three-dimensional (3D) simulations
0%
10%
20%
30%
40%
50%
60%
70%
80%
90%
100%
1 10 100 1000 10000
CO
2tr
app
ed
(%)
Time since injection starts (years)
超臨界CO2
残留CO2
溶存CO2
鉱物CO2
-1.0E+10
-5.0E+9
0.0E+0
5.0E+9
1.0E+10
1.5E+10
2.0E+10
1 10 100 1000 10000
Cha
ng
es in m
ine
ral a
bu
nd
an
ce
(mo
l)
Time since injection starts (years)
石英
非晶質シリカ
斜長石
カリ長石
方解石
シデライト
マグネサイト
ドーソナイト
ドロマイト
FeNa-サポナ
イトカオリナイト
緑泥石
海緑石
蛇紋石
黒雲母
黄鉄鉱
Na-斜プチロル
沸石
0%
10%
20%
30%
40%
50%
60%
70%
80%
90%
100%
1 10 100 1000 10000
CO
2tr
app
ed
(%)
Time since injection starts (years)
超臨界CO
2残留CO2
溶存CO2
鉱物CO2
-1.0E+10
-5.0E+9
0.0E+0
5.0E+9
1.0E+10
1.5E+10
2.0E+10
1 10 100 1000 10000
Cha
ng
es in m
inera
l a
bu
nd
an
ce
(mo
l)
Time since injection starts (years)
石英
非晶質シリカ
斜長石
カリ長石
方解石
シデライト
マグネサイト
ドーソナイト
ドロマイト
FeNa-サポナ
イトカオリナイト
緑泥石
海緑石
蛇紋石
黒雲母
黄鉄鉱
Na-斜プチロル
沸石
glauconite
amorph silica
siderite
calcite
kaolinite
magnesite
Moebetsu, inj-MN1(3D)
pyrite
aqueous
super-critical mineral
Moebetsu, inj-MN3(3D)
aqueous
super-critical
mineral
glauconite
amorph silica siderite
calcite
kaolinite
magnesite
precipitation
dissolution
precipitation
dissolution
residual trapped
chlorite
residual trapped
Reactive surface area of glauconite was reduced by 4 orders of magnitude for “inj-MN3”.
• Prominent reactions are same as 1D.• Mineral trapping of CO2 is similar
to 1D if dissolution of glauconite is fast.
• However, “inj-MN3” model with slow dissolution of glauconite is different from 1D over 1,000 years.
60% mineral trapped in “inj-MN3” model at 10,000 years
• Geochemical models were coupled with 3D field-scale reservoir model
• 3.6km×4km×800m• 43,119 active grids• 200,000 tons/year for 3 years• TOUGHREACT
10
3D field-scale simulations (molality & pH of inj-MN3 model)
K=41
I=10
K=41
I=10
(a)
(b)
(c)
(d)
North North
North North
Dissolved CO2 in water (molality) water pH
• Upward movement of CO2 driven by buoyancy forces is limited because much is trapped as residual CO2 .• Over 1,000 years, downward movement of water saturated with CO2, which is slightly denser than the original formation water, is predicted.
11
K=41
I=10
K=41
I=10
(e)
(f)
(g)
(h)
North North
North North
3D field-scale simulations (glauconite & siderite of inj-MN3 model)
Changes of glauconite (mol/m3) Changes of siderite (mol/m3)
• Gravity flow of the CO2 saturated water promotes mineral leaching and trapping over 1,000 years.
12
Conclusions
• We developed a geochemical model that successfully explains observed diagenesis and water composition.
• The reactive surface areas of minerals, generally unknown in the subsurface, were estimated based on the long-term stability of water composition.
• However, large uncertainties, in the orders of magnitude, still remain. We believe slow glauconite dissolution case is the most reasonable prediction as glauconite is abundant in the matrix of the sandstone.
• More information on reactive surface areas at in situ reservoir conditions is needed. • We also recognized that the geochemical simulation fully coupled with a three-
dimensional hydrodynamic model including residual trapping is important for the long-term assessment of the CO2 behavior.
13
Acknowledgements
This study was supported by the Ministry of Economy, Trade and Industry of Japan (METI), Japan CCS Co., Ltd. (JCCS) and Research Institute of Innovative Technology for the Earth (RITE). The authors would like to thank to all staff involved in the project.
14
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