Jinfeng Liu , Timotheus K.T. Wolterbeek , Christopher J. Spiers
{"title":"受控应力-压力-温度条件下破碎橄榄岩碳化过程中的体积响应和渗透性演变","authors":"Jinfeng Liu , Timotheus K.T. Wolterbeek , Christopher J. Spiers","doi":"10.1016/j.ijrmms.2024.105886","DOIUrl":null,"url":null,"abstract":"<div><p>Peridotites (olivine-rich rocks) naturally react with CO<sub>2</sub>-rich fluids to eventually form carbonates. Complete conversion involves incorporation of substantial amounts of CO<sub>2</sub>, which requires prolonged fluid flow. Yet, these reactions also cause a large increase in solid volume (63–84 %), raising questions on how they proceed in nature without this excess solid volume clogging fluid pathways. It has been suggested that reaction-driven fracture, caused by development of crystallization pressure, facilitates continual creation of new pathways, allowing reaction to advance. If indeed so, this could enable injection of industrially captured CO<sub>2</sub> into peridotites for permanent sequestration. However, such a fracturing mechanism has not been reproduced experimentally. Here, we report nine reactive flow-through experiments, performed on pre-compacted Åheim dunite powder (∼88 % olivine) inside a 1D oedometer vessel, to simultaneously measure axial deformation and permeability development. Tests were performed at 150 °C and effective axial stresses of 1–15 MPa. After initial flow measurements using deionized water at 10 MPa, during which permeability and deformation remained unchanged, the samples were exposed to inflow of reactive fluid. Samples subjected to CO<sub>2</sub>-saturated brine/water or NaHCO<sub>3</sub>-saturated solution showed minor compaction (0–0.38 %), while permeability decreased from 10<sup>−16</sup>-10<sup>−17</sup> to 10<sup>−20</sup>-10<sup>−21</sup> m<sup>2</sup>. Microstructural and chemical analyses demonstrate a drastic reduction in porosity of the reaction zone where carbonation occurred. A reference sample exposed to NaHSO<sub>4</sub> solution (acidification, but no carbonation) instead showed slightly increased permeability, from 3 × 10<sup>−17</sup> to 8.2 × 10<sup>−17</sup> m<sup>2</sup>, associated with 0.05 % compaction strain. Combined, the observations suggest dissolution of olivine at the grain contacts, leading to minor mechanical compaction, followed by precipitation of carbonates inside the remaining pores, clogging transport paths and thus reducing permeability. This indicates volume-increasing precipitation upon olivine carbonation under subsurface conditions clogs transport paths at laboratory timescales, severely limiting reaction rates and thus potential for crystallization pressure development and reaction-driven fracture.</p></div>","PeriodicalId":54941,"journal":{"name":"International Journal of Rock Mechanics and Mining Sciences","volume":"182 ","pages":"Article 105886"},"PeriodicalIF":7.0000,"publicationDate":"2024-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Volumetric response and permeability evolution during carbonation of crushed peridotite under controlled stress-pressure-temperature conditions\",\"authors\":\"Jinfeng Liu , Timotheus K.T. Wolterbeek , Christopher J. Spiers\",\"doi\":\"10.1016/j.ijrmms.2024.105886\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Peridotites (olivine-rich rocks) naturally react with CO<sub>2</sub>-rich fluids to eventually form carbonates. Complete conversion involves incorporation of substantial amounts of CO<sub>2</sub>, which requires prolonged fluid flow. Yet, these reactions also cause a large increase in solid volume (63–84 %), raising questions on how they proceed in nature without this excess solid volume clogging fluid pathways. It has been suggested that reaction-driven fracture, caused by development of crystallization pressure, facilitates continual creation of new pathways, allowing reaction to advance. If indeed so, this could enable injection of industrially captured CO<sub>2</sub> into peridotites for permanent sequestration. However, such a fracturing mechanism has not been reproduced experimentally. Here, we report nine reactive flow-through experiments, performed on pre-compacted Åheim dunite powder (∼88 % olivine) inside a 1D oedometer vessel, to simultaneously measure axial deformation and permeability development. Tests were performed at 150 °C and effective axial stresses of 1–15 MPa. After initial flow measurements using deionized water at 10 MPa, during which permeability and deformation remained unchanged, the samples were exposed to inflow of reactive fluid. Samples subjected to CO<sub>2</sub>-saturated brine/water or NaHCO<sub>3</sub>-saturated solution showed minor compaction (0–0.38 %), while permeability decreased from 10<sup>−16</sup>-10<sup>−17</sup> to 10<sup>−20</sup>-10<sup>−21</sup> m<sup>2</sup>. Microstructural and chemical analyses demonstrate a drastic reduction in porosity of the reaction zone where carbonation occurred. A reference sample exposed to NaHSO<sub>4</sub> solution (acidification, but no carbonation) instead showed slightly increased permeability, from 3 × 10<sup>−17</sup> to 8.2 × 10<sup>−17</sup> m<sup>2</sup>, associated with 0.05 % compaction strain. Combined, the observations suggest dissolution of olivine at the grain contacts, leading to minor mechanical compaction, followed by precipitation of carbonates inside the remaining pores, clogging transport paths and thus reducing permeability. This indicates volume-increasing precipitation upon olivine carbonation under subsurface conditions clogs transport paths at laboratory timescales, severely limiting reaction rates and thus potential for crystallization pressure development and reaction-driven fracture.</p></div>\",\"PeriodicalId\":54941,\"journal\":{\"name\":\"International Journal of Rock Mechanics and Mining Sciences\",\"volume\":\"182 \",\"pages\":\"Article 105886\"},\"PeriodicalIF\":7.0000,\"publicationDate\":\"2024-09-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Rock Mechanics and Mining Sciences\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S136516092400251X\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, GEOLOGICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Rock Mechanics and Mining Sciences","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S136516092400251X","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, GEOLOGICAL","Score":null,"Total":0}
Volumetric response and permeability evolution during carbonation of crushed peridotite under controlled stress-pressure-temperature conditions
Peridotites (olivine-rich rocks) naturally react with CO2-rich fluids to eventually form carbonates. Complete conversion involves incorporation of substantial amounts of CO2, which requires prolonged fluid flow. Yet, these reactions also cause a large increase in solid volume (63–84 %), raising questions on how they proceed in nature without this excess solid volume clogging fluid pathways. It has been suggested that reaction-driven fracture, caused by development of crystallization pressure, facilitates continual creation of new pathways, allowing reaction to advance. If indeed so, this could enable injection of industrially captured CO2 into peridotites for permanent sequestration. However, such a fracturing mechanism has not been reproduced experimentally. Here, we report nine reactive flow-through experiments, performed on pre-compacted Åheim dunite powder (∼88 % olivine) inside a 1D oedometer vessel, to simultaneously measure axial deformation and permeability development. Tests were performed at 150 °C and effective axial stresses of 1–15 MPa. After initial flow measurements using deionized water at 10 MPa, during which permeability and deformation remained unchanged, the samples were exposed to inflow of reactive fluid. Samples subjected to CO2-saturated brine/water or NaHCO3-saturated solution showed minor compaction (0–0.38 %), while permeability decreased from 10−16-10−17 to 10−20-10−21 m2. Microstructural and chemical analyses demonstrate a drastic reduction in porosity of the reaction zone where carbonation occurred. A reference sample exposed to NaHSO4 solution (acidification, but no carbonation) instead showed slightly increased permeability, from 3 × 10−17 to 8.2 × 10−17 m2, associated with 0.05 % compaction strain. Combined, the observations suggest dissolution of olivine at the grain contacts, leading to minor mechanical compaction, followed by precipitation of carbonates inside the remaining pores, clogging transport paths and thus reducing permeability. This indicates volume-increasing precipitation upon olivine carbonation under subsurface conditions clogs transport paths at laboratory timescales, severely limiting reaction rates and thus potential for crystallization pressure development and reaction-driven fracture.
期刊介绍:
The International Journal of Rock Mechanics and Mining Sciences focuses on original research, new developments, site measurements, and case studies within the fields of rock mechanics and rock engineering. Serving as an international platform, it showcases high-quality papers addressing rock mechanics and the application of its principles and techniques in mining and civil engineering projects situated on or within rock masses. These projects encompass a wide range, including slopes, open-pit mines, quarries, shafts, tunnels, caverns, underground mines, metro systems, dams, hydro-electric stations, geothermal energy, petroleum engineering, and radioactive waste disposal. The journal welcomes submissions on various topics, with particular interest in theoretical advancements, analytical and numerical methods, rock testing, site investigation, and case studies.