Study of corrosion mechanism of dawsonite led by CO<sub>2</sub> partial pressure

doi:10.1007/s11707-021-0901-1

Front. Earth Sci.

2022, Vol. 16

Issue (2) : 465-482 https://doi.org/10.1007/s11707-021-0901-1

RESEARCH ARTICLE

Study of corrosion mechanism of dawsonite led by CO₂ partial pressure

Fulai LI^1,²(

), Hao DIAO^1,², Wenkuan MA^1,², Maozhen WANG³

¹. Shandong Provincial Key Laboratory of Deep Oil and Gas, School of Geosciences, China University of Petroleum (East China), Qingdao 266580, China
². Laboratory for Marine Mineral Resources, Qingdao National Laboratory for Marine Science and Technology, Qingdao 266071, China
³. Bohai Oilfield Research Institute, Tianjin Branch of CNOOC China Limited, Tianjin 300452, China

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Abstract

The stability of dawsonite is an important factor affecting the feasibility evaluation of CO₂ geological storage. In this paper, a series of experiments on the interaction of CO₂-water-dawsonite-bearing sandstone were carried out under different CO₂ pressures. Considering the dissolution morphology and element composition of dawsonite after the experiment and the fluid evolution in equilibrium with dawsonite, the corrosion mechanism of dawsonite led by CO₂ partial pressure was discussed. The CO₂ fugacity of the vapor phase in the system was calculated using the Peng–Robinson equation of state combined with the van der Waals 1-fluid mixing rule. The experimental results indicated that the thermodynamic stability of dawsonite increased with the increase of CO₂ partial pressure and decreased with the increase of temperature. The temperature at which dawsonite dissolution occurred was higher at higher $f C O 2$ . There were two different ways to reduce dawsonite’s stability: the transformation of constituent elements and crystal structure damage. Dawsonite undergoes component element transformation and crystal structure damage under different CO₂ pressures with certain temperature limits. Based on the comparison of the corrosion temperature of dawsonite, three corrosion evolution models of dawsonite under low, medium, and high CO₂ pressures were summarized. Under conditions of medium and low CO₂ pressure, as the temperature continued to increase and exceeded its stability limit, the dawsonite crystal structure was corroded first. Then the constituent elements of dawsonite dissolved, and the transformation of dawsonite to gibbsite began. At high CO₂ pressure, the constituent elements of dawsonite dissolved first with the increase of temperature, forming gibbsite, followed by the corrosion of crystalline structure.

Keywords dawsonite stability CO₂-water-rock interaction corrosion mechanism CO₂ geological storage

Corresponding Author(s): Fulai LI

About author: Tongcan Cui and Yizhe Hou contributed equally to this work.

Online First Date: 19 October 2021 Issue Date: 26 August 2022

Cite this article:

Fulai LI,Hao DIAO,Wenkuan MA, et al. Study of corrosion mechanism of dawsonite led by CO₂ partial pressure[J]. Front. Earth Sci., 2022, 16(2): 465-482.

URL:

https://academic.hep.com.cn/fesci/EN/10.1007/s11707-021-0901-1
https://academic.hep.com.cn/fesci/EN/Y2022/V16/I2/465

Fig.1 Laboratory apparatus used for water-rock-CO₂ reactions.

Tab.1 Initial reaction conditions and weight loss of samples

Fig.2 Mass loss ratio of sandstone samples. (a) Mass loss ratio of sandstone samples at normal pressure; (b) mass loss ratio of sandstone samples at 4 MPa; (c) mass loss ratio of sandstone samples at 7.3 MPa.

Fig.3 Mineral composition of sandstone samples. (a) Mineral contents of the original sandstone sample; (b) the content of each mineral in the sandstone sample at normal pressure 80°C; (c) the content of each mineral in the sandstone sample at normal pressure 100°C; (d) the content of each mineral in the sandstone sample at 4 MPa 80°C; (e) the content of each mineral in the sandstone sample at 4 MPa 100°C; (f) the content of each mineral in the sandstone sample at 4 MPa 120°C; (g) the content of each mineral in the sandstone sample at 7.3 MPa 120°C; (h) the content of each mineral in the sandstone sample at 7.3 MPa 140°C; (i) the content of each mineral in the sandstone sample at 7.3 MPa 160°C.

Tab.2 Concentration of soluble species in solutions after reactions

Fig.4 Ion dissolution rate of each anion and cation in the solution after the reaction. (a) The change of anionic ion dissolution rate with temperature in the reaction solution at normal pressure; (b) the change of cationic ion dissolution rate with temperature in the reaction solution at normal pressure; (c) the change of anionic ion dissolution rate with temperature in the reaction solution at 4 MPa; (d) the change of cationic ion dissolution rate with temperature in the reaction solution at 4 MPa; (e) the change of anionic ion dissolution rate with temperature in the reaction solution at 7.3 MPa; (f) the change of cationic ion dissolution rate with temperature in the reaction solution at 7.3 MPa.

Fig.5 SEM photos of erosion and dissolution of major minerals in sandstone. (a) Calcite eroded along cleavages, and the surface was eroded to form a large number of pits and channels (normal pressure, T= 80°C); (b) kaolinite is vermiform and only slightly eroded (normal pressure, T= 80°C); (c) slight dissolution of potassium feldspar resulted in tiny pores on the mineral surface and tiny channels along cleavages (normal pressure, T = 100°C); (d) the further dissolution of potassium feldspar, corrosion pits increased, the hole deepened (P = 4 MPa, T= 80°C); (e) albite is obviously eroded, with wide and long channels and large holes on the surface (P = 4 MPa, T = 100°C); (f) the surface of quartz grains is smooth (P = 4 MPa, T = 120°C); (g) illite is reticular and slightly corroded (P = 7.3 MPa, T = 120°C); (h) albite is severely eroded, and the mineral has completely dissolved locally, leaving only some of the residue along the cleavage (P = 7.3 MPa, T= 140°C); (i) dissolution of potassium feldspar, the mineral surface was dissolved along the cleavages and formed a staggered channel (P = 7.3 MPa, T= 160°C). Cal-calcite, kln-kaolinite, kfs-potassium feldspar, Ab-albite, Qtz-quartz, Ill-illite.

Fig.6 SEM photos of dawsonite under different experimental conditions. (a) SEM photo of dawsonite in original sandstone; (b) dawsonite eroded significantly, and the surface of the columnar crystal became extremely rough, forming a large number of craters (normal pressure, T= 80°C); (c) dawsonite was further corroded into a thorn shape and the degree of dissolution of dawsonite aggregate was enhanced from the root to the outer edge (normal pressure, T= 100°C); (d) dawsonite preserved well and the mineral surface is relatively regular (P = 4 MPa, T = 80°C); (e) dawsonite with no obvious corrosion (P = 4 MPa, T= 100°C); (f) the surface of dawsonite was dissolved, the edges of the crystal were no longer clear, and the surface was covered by newly precipitated minerals (P = 4 MPa, T= 120°C); (g) the shape of dawsonite aggregate remained intact, but the crystal edges were no longer distinct and the surface was attached by fine new minerals (P = 7.3 MPa, T = 120°C); (h) radial dawsonite aggregate, the edges of individual crystals were more blurred, and the columnar shape was further lost (P = 7.3 MPa, T= 140°C); (i) dawsonite crystals were almost completely turned grayish white, and the aggregates dissolved from the outer edge of the columnar crystal to the root (P = 7.3 MPa, T = 160°C).

Fig.7 The composition and content evolution of dawsonite. (a) SEM photo of dawsonite in original sample, and the energy spectrum at the marked point; (b) SEM photo of dawsonite in sandstone at normal pressure 80°C, and the energy spectrum at the marked point; (c) SEM photo of dawsonite in sandstone at normal pressure 100°C, and the energy spectrum at the marked point; (d) the content of dawsonite under the experiment of normal pressure; (e) SEM photo of dawsonite in sandstone at 4 MPa 80°C, and the energy spectrum at the marked point; (f) SEM photo of dawsonite in sandstone at 4 MPa 100°C, and the energy spectrum at the marked point; (g) SEM photo of dawsonite in sandstone at 4 MPa 120°C, and the energy spectrum at the marked point; (h) the content of dawsonite under the experimental pressure of 4 MPa; (i) SEM photo of dawsonite in sandstone at 7.3 MPa 120°C, and the energy spectrum at the marked point; (j) SEM photo of dawsonite in sandstone at 7.3 MPa 140°C, and the energy spectrum at the marked point; (k) SEM photo of dawsonite in sandstone at 7.3 MPa 160°C, and the energy spectrum at the marked point; (h) the content of dawsonite under the experimental pressure of 7.3 MPa.

P/MPa	T/K	x		P_c/MPa		T_c/K		ω		k₁₂	$f C O 2$ /MPa
P/MPa	T/K	CO₂	H₂O	CO₂	H₂O	CO₂	H₂O	CO₂	H₂O	k₁₂	$f C O 2$ /MPa
4	353.15	0.984	0.016	7.383	22.048	304.21	647.30	0.2236	0.3442	0.165	3.9
4	373.15	0.968	0.032	7.383	22.048	304.21	647.30	0.2236	0.3442	0.165	3.8
4	393.15	0.939	0.061	7.383	22.048	304.21	647.30	0.2236	0.3442	0.165	3.7
7.3	393.15	0.959	0.041	7.383	22.048	304.21	647.30	0.2236	0.3442	0.165	6.9
7.3	413.15	0.931	0.069	7.383	22.048	304.21	647.30	0.2236	0.3442	0.165	6.7
7.3	433.15	0.887	0.113	7.383	22.048	304.21	647.30	0.2236	0.3442	0.165	6.4

Tab.3 The parameters used for the calculation and the corrected CO₂ fugacity values

Fig.8 Elemental composition evolution of dawsonite after the reaction.

Fig.9 Dissolution patterns of dawsonite under different CO₂ partial pressures and temperature conditions.

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