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Geological and Mineralogical Sequestration of CO₂

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A special issue of Minerals (ISSN 2075-163X).

Deadline for manuscript submissions: closed (31 July 2019) | Viewed by 41915

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Special Issue Editors

Dr. Giovanni Ruggieri

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Guest Editor

Istituto di Geoscienze e Georisorse–CNR, U.O.S. di Firenze, 50121 Firenze, Italy
Interests: fluid inclusions; stable isotopes; CO₂ mineral sequestration; geothermal resources; hydrothermal mineralization; fluid-rock interaction experiments; ore deposits
Special Issues, Collections and Topics in MDPI journals

Dr. Fabrizio Gherardi

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Guest Editor

Istituto di Geoscienze e Georisorse–CNR, 56124 Pisa, Italy
Interests: fluid geochemistry; isotope hydrology; gas–water–rock interactions; geochemical/reactive transport modeling; CO₂ geological storage; geothermal resources

Special Issue Information

Dear Colleagues,

The rapid increase of concentrations of greenhouse gases, anthropologically-generated (primarily CO₂) in the atmosphere, is responsible for global warming and ocean acidification. Carbon capture and storage (CCS) techniques have been proposed and developed to contrast the rise of CO₂ in atmosphere. One of the technological solutions is the long-term storage of CO₂ into appropriate geological formations, such as deep saline formations and depleted oil and gas reservoirs. A potential alternative to CO₂ geological storage is CO₂ mineral sequestration through carbonation (ex situ and in situ), leading to the permanent and safe storage of CO₂.

This Special Issue aims to collect articles covering various aspects of recent scientific advances of CO₂ storage, including characterization of storage formations and cap-rocks and their behavior during CO₂ injection, storage modelling studies for test design, test site results and environmental monitoring, numerical modelling of geochemical-mineralogical reactions and CO₂ flow, studies of natural analogs of CO₂ storage and CO₂ mineral sequestration, and experimental investigations to better understand long-term geological storage and carbonation processes.

Dr. Giovanni Ruggieri
Dr. Fabrizio Gherardi
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Minerals is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2400 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

Geological CO₂ storage
CO₂ storage test-site
Mineral carbonation
Numerical modeling
Fluid-rock interaction experiments
Natural analogues of CO₂ storage

Published Papers (11 papers)

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Editorial

Jump to: Research

4 pages, 176 KiB

Open AccessEditorial

Editorial for Special Issue “Geological and Mineralogical Sequestration of CO₂”

by Giovanni Ruggieri and Fabrizio Gherardi

Minerals 2020, 10(7), 603; https://doi.org/10.3390/min10070603 - 02 Jul 2020

Cited by 2 | Viewed by 1575

Abstract

Carbon Capture Utilization and Storage (CCUS) has been substantiated by the International Panel on Climate Change (IPCC) [...] Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

Research

Jump to: Editorial

24 pages, 5385 KiB

Open AccessArticle

Low Temperature Serpentinite Replacement by Carbonates during Seawater Influx in the Newfoundland Margin

by Suzanne Picazo, Benjamin Malvoisin, Lukas Baumgartner and Anne-Sophie Bouvier

Minerals 2020, 10(2), 184; https://doi.org/10.3390/min10020184 - 18 Feb 2020

Cited by 15 | Viewed by 4725

Abstract

Serpentinite replacement by carbonates in the seafloor is one of the main carbonation processes in nature providing insights into the mechanisms of CO₂ sequestration; however, the onset of this process and the conditions for the reaction to occur are not yet fully understood. Preserved serpentine rim with pseudomorphs of carbonate after serpentine and lobate-shaped carbonate grains are key structural features for replacement of serpentinite by carbonates. Cathodoluminescence microscopy reveals that Ca-rich carbonate precipitation in serpentinite is associated with a sequential assimilation of Mn. Homogeneous δ¹⁸O values at the µm-scale within grains and host sample indicate low formation temperature (<20 °C) from carbonation initiation, with a high fluid to rock ratio. δ¹³C (1–3 ± 1‰) sit within the measured values for hydrothermal systems (−3–3‰), with no systematic correlation with the Mn content. δ¹³C values reflect the inorganic carbon dominance and the seawater source of CO₂ for carbonate. Thermodynamic modeling of fluid/rock interaction during seawater transport in serpentine predicts Ca-rich carbonate production, at the expense of serpentine, only at temperatures below 50 °C during seawater influx. Mg-rich carbonates can also be produced when using a model of fluid discharge, but at significantly higher temperatures (150 °C). This has major implications for the setting of carbonation in present-day and in fossil margins. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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18 pages, 7147 KiB

Open AccessFeature PaperArticle

Spontaneous Serpentine Carbonation Controlled by Underground Dynamic Microclimate at the Montecastelli Copper Mine, Italy

by Chiara Boschi, Federica Bedini, Ilaria Baneschi, Andrea Rielli, Lukas Baumgartner, Natale Perchiazzi, Alexey Ulyanov, Giovanni Zanchetta and Andrea Dini

Minerals 2020, 10(1), 1; https://doi.org/10.3390/min10010001 - 18 Dec 2019

Cited by 5 | Viewed by 2967

Abstract

Understanding low temperature carbon sequestration through serpentinite–H₂O–CO₂ interaction is becoming increasingly important as it is considered a potential approach for carbon storage required to offset anthropogenic CO₂ emissions. In this study, we present new insights into spontaneous CO₂ mineral sequestration through the formation of hydromagnesite + kerolite with minor aragonite incrustations on serpentinite walls of the Montecastelli copper mine located in Southern Tuscany, Italy. On the basis of field, petrological, and geochemical observations coupled with geochemical modeling, we show that precipitation of the wall coating paragenesis is driven by a sequential evaporation and condensation process starting from meteoric waters which emerge from fractures into the mine walls and ceiling. A direct precipitation of the coating paragenesis is not compatible with the chemical composition of the mine water. Instead, geochemical modeling shows that its formation can be explained through evaporation of mine water and its progressive condensation onto the mine walls, where a layer of serpentinite powder was accumulated during the excavation of the mine adits. Condensed water produces a homogeneous film on the mine walls where it can interact with the serpentinite powder and become enriched in Mg, Si, and minor Ca, which are necessary for the precipitation of the observed coating paragenesis. The evaporation and condensation processes are driven by changes in the air flow inside the mine, which in turns are driven by seasonal changes of the outside temperature. The presence of “kerolite”, a Mg-silicate, is indicative of the dissolution of Si-rich minerals, such as serpentine, through the water–powder interaction on the mine walls at low temperature (~17.0 to 18.1 °C). The spontaneous carbonation of serpentine at low temperature is a peculiar feature of this occurrence, which has only rarely been observed in ultramafic outcrops exposed on the Earth’s surface, where instead hydromagnesite predominantly forms through the dissolution of brucite. The high reactivity of serpentine observed, in this study, is most likely due to the presence of fine-grained serpentine fines in the mine walls. Further study of the peculiar conditions of underground environments hosted in Mg-rich lithologies, such as that of the Montecastelli Copper mine, can lead to a better understanding of the physical and chemical conditions necessary to enhance serpentine carbonation at ambient temperature. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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14 pages, 1067 KiB

Open AccessEditor’s ChoiceArticle

Mineralogical Transformations of Heated Serpentine and Their Impact on Dissolution during Aqueous-Phase Mineral Carbonation Reaction in Flue Gas Conditions

by Clémence Du Breuil, Louis César-Pasquier, Gregory Dipple, Jean-François Blais, Maria Cornelia Iliuta and Guy Mercier

Minerals 2019, 9(11), 680; https://doi.org/10.3390/min9110680 - 03 Nov 2019

Cited by 11 | Viewed by 4311

Abstract

Mineral carbonation is known to be among the most efficient ways to reduce the anthropogenic emissions of carbon dioxide. Serpentine minerals (Mg₃Si₂O₅(OH)₄), have shown great potential for carbonation. A way to improve yield is to thermally activate serpentine minerals prior to the carbonation reaction. This step is of great importance as it controls Mg²⁺ leaching, one of the carbonation reaction limiting factors. Previous studies have focused on the optimization of the thermal activation by determining the ideal activation temperature. However, to date, none of these studies have considered the impacts of the thermal activation on the efficiency of the aqueous-phase mineral carbonation at ambient temperature and moderate pressure in flue gas conditions. Several residence times and temperatures of activation have been tested to evaluate their impact on serpentine dissolution in conditions similar to mineral carbonation. The mineralogical composition of the treated solids has been studied using X-ray diffraction coupled with a quantification using the Rietveld refinement method. A novel approach in order to quantify the meta-serpentine formed during dehydroxylation is introduced. The most suitable mineral assemblage for carbonation is found to be a mixture of the different amorphous phases identified. This study highlights the importance of the mineralogical assemblage obtained during the dehydroxylation process and its impact on the magnesium availability during dissolution in the carbonation reaction. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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23 pages, 6218 KiB

Open AccessArticle

Using Reservoir Geology and Petrographic Observations to Improve CO₂ Mineralization Estimates: Examples from the Johansen Formation, North Sea, Norway

by Anja Sundal and Helge Hellevang

Minerals 2019, 9(11), 671; https://doi.org/10.3390/min9110671 - 31 Oct 2019

Cited by 16 | Viewed by 5009

Abstract

Reservoir characterization specific to CO₂ storage is challenging due to the dynamic interplay of physical and chemical trapping mechanisms. The mineralization potential for CO₂ in a given siliciclastic sandstone aquifer is controlled by the mineralogy, the total reactive surface areas, and the prevailing reservoir conditions. Grain size, morphologies and mineral assemblages vary according to sedimentary facies and diagenetic imprint. The proposed workflow highlights how the input values for reactive mineral surface areas used in geochemical modelling may be parameterized as part of geological reservoir characterization. The key issue is to separate minerals both with respect to phase chemistry and morphology (i.e., grain size, shape, and occurrence), and focus on main reactants for sensitivity studies and total storage potentials. The Johansen Formation is the main reservoir unit in the new full-value chain CO₂ capture and storage (CCS) prospect in Norway, which was licenced for the storage of CO₂ as of 2019. The simulations show how reaction potentials vary in different sedimentary facies and for different mineral occurrences. Mineralization potentials are higher in fine-grained facies, where plagioclase and chlorite are the main cation donors for carbonatization. Reactivity decreases with higher relative fractions of ooidal clay and lithic fragments. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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15 pages, 4047 KiB

Open AccessArticle

Injection of a CO₂-Reactive Solution for Wellbore Annulus Leakage Remediation

by Laura Wasch and Mariëlle Koenen

Minerals 2019, 9(10), 645; https://doi.org/10.3390/min9100645 - 22 Oct 2019

Cited by 8 | Viewed by 2940

Abstract

Driven by concerns for safe storage of CO₂, substantial effort has been directed on wellbore integrity simulations over the last decade. Since large scale demonstrations of CO₂ storage are planned for the near-future, numerical tools predicting wellbore integrity at field scale are essential to capture the processes of potential leakage and assist in designing leakage mitigation measures. Following this need, we developed a field-scale wellbore model incorporating (1) a de-bonded interface between cement and rock, (2) buoyancy/pressure driven (microannulus) flow of brine and CO₂, (3) CO₂ diffusion and reactivity with cement and (4) chemical cement-rock interaction. The model is aimed at predicting leakage through the microannulus and specifically at assessing methods for CO₂ leakage remediation. The simulations show that for a low enough initial leakage rate, CO₂ leakage is self-limiting due to natural sealing of the microannulus by mineral precipitation. With a high leakage rate, CO₂ leakage results in progressive cement leaching. In case of sustained leakage, a CO₂ reactive solution can be injected in the microannulus to induce calcite precipitation and block the leak path. The simulations showed full clogging of the leak path and increased sealing with time after remediation, indicating the robustness of the leakage remediation by mineral precipitation. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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17 pages, 3622 KiB

Open AccessArticle

Potential for Mineral Carbonation of CO₂ in Pleistocene Basaltic Rocks in Volos Region (Central Greece)

by Nikolaos Koukouzas, Petros Koutsovitis, Pavlos Tyrologou, Christos Karkalis and Apostolos Arvanitis

Minerals 2019, 9(10), 627; https://doi.org/10.3390/min9100627 - 11 Oct 2019

Cited by 15 | Viewed by 5806

Abstract

Pleistocene alkaline basaltic lavas crop out in the region of Volos at the localities of Microthives and Porphyrio. Results from detailed petrographic study show porphyritic textures with varying porosity between 15% and 23%. Data from deep and shallow water samples were analysed and belong to the Ca-Mg-Na-HCO₃-Cl and the Ca-Mg-HCO₃ hydrochemical types. Irrigation wells have provided groundwater temperatures reaching up to ~30 °C. Water samples obtained from depths ranging between 170 and 250 m. The enhanced temperature of the groundwater is provided by a recent-inactive magmatic heating source. Comparable temperatures are also recorded in adjacent regions in which basalts of similar composition and age crop out. Estimations based on our findings indicate that basaltic rocks from the region of Volos have the appropriate physicochemical properties for the implementation of a financially feasible CO₂ capture and storage scenario. Their silica-undersaturated alkaline composition, the abundance of Ca-bearing minerals, low alteration grade, and high porosity provide significant advantages for CO₂ mineral carbonation. Preliminary calculations suggest that potential pilot projects at the Microthives and Porphyrio basaltic formations can store 64,800 and 21,600 tons of CO₂, respectively. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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14 pages, 4373 KiB

Open AccessArticle

Proposed Methodology to Evaluate CO₂ Capture Using Construction and Demolition Waste

by Domingo Martín, Vicente Flores-Alés and Patricia Aparicio

Minerals 2019, 9(10), 612; https://doi.org/10.3390/min9100612 - 05 Oct 2019

Cited by 16 | Viewed by 3290

Abstract

Since the Industrial Revolution, levels of CO₂ in the atmosphere have been constantly growing, producing an increase in the average global temperature. One of the options for Carbon Capture and Storage is mineral carbonation. The results of this process of fixing are the safest in the long term, but the main obstacle for mineral carbonation is the ability to do it economically in terms of both money and energy cost. The present study outlines a methodological sequence to evaluate the possibility for the carbonation of ceramic construction waste (brick, concrete, tiles) under surface conditions for a short period of time. The proposed methodology includes a pre-selection of samples using the characterization of chemical and mineralogical conditions and in situ carbonation. The second part of the methodology is the carbonation tests in samples selected at 10 and 1 bar of pressure. The relative humidity during the reaction was 20 wt %, and the reaction time ranged from 24 h to 30 days. To show the effectiveness of the proposed methodology, Ca-rich bricks were used, which are rich in silicates of calcium or magnesium. The results of this study showed that calcite formation is associated with the partial destruction of Ca silicates, and that carbonation was proportional to reaction time. The calculated capture efficiency was proportional to the reaction time, whereas carbonation did not seem to significantly depend on particle size in the studied conditions. The studies obtained at a low pressure for the total sample were very similar to those obtained for finer fractions at 10 bars. Presented results highlight the utility of the proposed methodology. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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18 pages, 3341 KiB

Open AccessEditor’s ChoiceArticle

Experimental Simulation of the Self-Trapping Mechanism for CO₂ Sequestration into Marine Sediments

by Hak-Sung Kim and Gye-Chun Cho

Minerals 2019, 9(10), 579; https://doi.org/10.3390/min9100579 - 24 Sep 2019

Cited by 8 | Viewed by 3085

Abstract

CO₂ hydrates are ice-like solid lattice compounds composed of hydrogen-bonded cages of water molecules that encapsulate guest CO₂ molecules. The formation of CO₂ hydrates in unconsolidated sediments significantly decreases their permeability and increases their stiffness. CO₂ hydrate-bearing sediments can, therefore, act as cap-rocks and prevent CO₂ leakage from a CO₂-stored layer. In this study, we conducted an experimental simulation of CO₂ geological storage into marine unconsolidated sediments. CO₂ hydrates formed during the CO₂ liquid injection process and prevented any upward flow of CO₂. Temperature, pressure, P-wave velocity, and electrical resistance were measured during the experiment, and their measurement results verified the occurrence of the self-trapping effect induced by CO₂ hydrate formation. Several analyses using the experimental results revealed that CO₂ hydrate bearing-sediments have a considerable sealing capacity. Minimum breakthrough pressure and maximum absolute permeability are estimated to be 0.71 MPa and 5.55 × 10⁻⁴ darcys, respectively. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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21 pages, 7571 KiB

Open AccessArticle

Potential for the Geological Storage of CO₂ in the Croatian Part of the Adriatic Offshore

by Bruno Saftić, Iva Kolenković Močilac, Marko Cvetković, Domagoj Vulin, Josipa Velić and Bruno Tomljenović

Minerals 2019, 9(10), 577; https://doi.org/10.3390/min9100577 - 23 Sep 2019

Cited by 6 | Viewed by 4499

Abstract

Every country with a history of petroleum exploration has acquired geological knowledge of its sedimentary basins and might therefore make use of a newly emerging resource—as there is the potential to decarbonise energy and industry sectors by geological storage of CO₂. To reduce its greenhouse gas emissions and contribute to meeting the Paris agreement targets, Croatia should map this potential. The most prospective region is the SW corner of the Pannonian basin, but there are also offshore opportunities in the Northern and Central Adriatic. Three “geological storage plays” are suggested for detailed exploration in this province. Firstly, there are three small gas fields (Ida, Ika and Marica) with Pliocene and Pleistocene reservoirs suitable for storage and they can be considered as the first option, but only upon expected end of production. Secondly, there are Miocene sediments in the Dugi otok basin whose potential is assessed herein as a regional deep saline aquifer. The third option would be to direct future exploration to anticlines composed of carbonate rocks with primary and secondary porosity, covered with impermeable Miocene to Holocene clastic sediments. Five closed structures of this type were contoured with a large total potential, but data on their reservoir properties allow only theoretical storage capacity estimates at this stage. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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14 pages, 2633 KiB

Open AccessArticle

Estimates of scCO₂ Storage and Sealing Capacity of the Janggi Basin in Korea Based on Laboratory Scale Experiments

by Jinyoung Park, Minjune Yang, Seyoon Kim, Minhee Lee and Sookyun Wang

Minerals 2019, 9(9), 515; https://doi.org/10.3390/min9090515 - 26 Aug 2019

Cited by 8 | Viewed by 2823

Abstract

Laboratory experiments were performed to measure the supercritical CO₂ (scCO₂) storage ratio (%) of conglomerate and sandstone in the Janggi Basin, which are classified as rock in Korea that are available for CO₂ storage. The scCO₂ storage capacity was evaluated by direct measurement of the amount of scCO₂ replacing the pore water in each reservoir rock core. The scCO₂ sealing capacity of the cap rock (i.e., tuff and mudstone) was also compared by measuring the scCO₂ capillary entry pressure (Δp) into the rock core. The measured average scCO₂ storage ratio of the conglomerate and the sandstone were 30.7% and 13.1%, respectively, suggesting that the scCO₂ storage capacity was greater than 360,000 metric tons. The scCO₂ capillary entry pressure for the tuff ranged from 15 to 20 bar and for the mudstone it was higher than 150 bar, suggesting that the mudstone layers had enough sealing capacity from the aspect of hydromechanics. From XRF analyses, before and after 90 d of the scCO₂-water-cap rock reaction, the mudstone and the tuff were investigated to assure their geochemical stability as the cap rock. From the study, the Janggi Basin was considered an optimal CO₂ storage site based on both its high scCO₂ storage ratio and high capillary entry pressure. Full article

(This article belongs to the Special Issue Geological and Mineralogical Sequestration of CO₂)

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