Complex carbonate phases drive geologic CO2 mineralization

Lahiri, Nabajit; Kovarik, Libor; Taylor, Sandra D.; Crum, Jarrod V.; Ilton, Eugene S.; Depp, Charles T.; Miller, Quin R. S.; Schaef, H. Todd

doi:10.1038/s43247-025-02273-6

Complex carbonate phases drive geologic CO₂ mineralization

Journal Article · Fri May 16 00:00:00 EDT 2025 · Communications Earth & Environment

DOI:https://doi.org/10.1038/s43247-025-02273-6· OSTI ID:2566948

^[1]; Kovarik, Libor ^[1]; ^[1]; ^[1]; Ilton, Eugene S. ^[1]; ^[2]; ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Colorado School of Mines, Golden, CO (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Geologic carbon sequestration in mafic and ultramafic reservoirs is a scalable strategy for carbon dioxide removal, offering permanent storage via mineralization as stable carbonates. However, there is limited information on the structure and composition of key mineralization endpoints during sequestration. Here, we unravel the atomic structure, composition, and nanoscale morphology of carbonates recovered from a field-scale demonstration of CO₂ mineralization in basalt. Using transmission electron microscopy, we mapped mineralogical variations from the initial to later stages of subsurface carbonate growth and identified a previously unknown cation-ordered ankerite phase that exerts a primary control over carbonation processes. This study has provided a new understanding of subsurface carbonation pathways which will impact the parameterization of predictive geochemical models for future sequestration efforts in basalt formations.

View Journal Article

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2566948

Alternate ID(s):: OSTI ID: 2570358

Report Number(s):: PNNL-SA--194276

Journal Information:: Communications Earth & Environment, Journal Name: Communications Earth & Environment Journal Issue: 1 Vol. 6; ISSN 2662-4435

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Visualizing the Atomic Configuration of Carbonate Groups in a (Cu,C)Ba₂Ca₃Cu₄O_11+δ Superconductor Lin, Renju; Wang, Qing; Song, Dongsheng Advanced Materials, Vol. 35, Issue 26 https://doi.org/10.1002/adma.202301021	journal	May 2023
Synthesis of the new compound CaFe(CO3)2 and experimental constraints on the (Ca,Fe)CO3 join Davidson, Paula M.; Symmes, Gregory H.; Cohen, Barbara A. Geochimica et Cosmochimica Acta, Vol. 57, Issue 23-24 https://doi.org/10.1016/0016-7037(93)90612-Z	journal	December 1993
Dissolution of Columbia River Basalt under mildly acidic conditions as a function of temperature: Experimental results relevant to the geological sequestration of carbon dioxide Todd Schaef, H.; Peter McGrail, B. Applied Geochemistry, Vol. 24, Issue 5 https://doi.org/10.1016/j.apgeochem.2009.02.025	journal	May 2009
Injection and Monitoring at the Wallula Basalt Pilot Project McGrail, B. P.; Spane, F. A.; Amonette, J. E. Energy Procedia, Vol. 63 https://doi.org/10.1016/j.egypro.2014.11.316	journal	January 2014
Inorganic synthesis of Fe–Ca–Mg carbonates at low temperature Romanek, Christopher S.; Jiménez-López, Concepción; Navarro, Alejandro Rodriguez Geochimica et Cosmochimica Acta, Vol. 73, Issue 18 https://doi.org/10.1016/j.gca.2009.05.065	journal	September 2009
An experimental study of basaltic glass–H2O–CO2 interaction at 22 and 50°C: Implications for subsurface storage of CO2 Galeczka, Iwona; Wolff-Boenisch, Domenik; Oelkers, Eric H. Geochimica et Cosmochimica Acta, Vol. 126 https://doi.org/10.1016/j.gca.2013.10.044	journal	February 2014
Reaction path modelling of in-situ mineralisation of CO2 at the CarbFix site at Hellisheidi, SW-Iceland Snæbjörnsdóttir, Sandra Ó.; Gislason, Sigurdur R.; Galeczka, Iwona M. Geochimica et Cosmochimica Acta, Vol. 220 https://doi.org/10.1016/j.gca.2017.09.053	journal	January 2018
New insights into Mn2+ and Mg2+ inhibition of calcite growth Mills, Jennifer V.; Barnhart, Holly A.; DePaolo, Donald J. Geochimica et Cosmochimica Acta, Vol. 334 https://doi.org/10.1016/j.gca.2022.06.015	journal	October 2022
Carbonate mineralization of volcanic province basalts Schaef, H. T.; McGrail, B. P.; Owen, A. T. International Journal of Greenhouse Gas Control, Vol. 4, Issue 2 https://doi.org/10.1016/j.ijggc.2009.10.009	journal	March 2010
Insights into silicate carbonation processes in water-bearing supercritical CO2 fluids Miller, Q. R. S.; Thompson, C. J.; Loring, J. S. International Journal of Greenhouse Gas Control, Vol. 15 https://doi.org/10.1016/j.ijggc.2013.02.005	journal	July 2013
On the evolution of dolomite stoichiometry and cation order during high-temperature synthesis experiments: An alternative model for the geochemical evolution of natural dolomites Kaczmarek, Stephen E.; Sibley, Duncan F. Sedimentary Geology, Vol. 240, Issue 1-2 https://doi.org/10.1016/j.sedgeo.2011.07.003	journal	August 2011
Phase contrast STEM for thin samples: Integrated differential phase contrast Lazić, Ivan; Bosch, Eric G. T.; Lazar, Sorin Ultramicroscopy, Vol. 160 https://doi.org/10.1016/j.ultramic.2015.10.011	journal	January 2016
Quantification of CO ₂ Mineralization at the Wallula Basalt Pilot Project White, Signe K.; Spane, Frank A.; Schaef, H. Todd Environmental Science & Technology, Vol. 54, Issue 22 https://doi.org/10.1021/acs.est.0c05142	journal	September 2020
Exotic Carbonate Mineralization Recovered from a Deep Basalt Carbon Storage Demonstration Polites, Ellen G.; Schaef, H. Todd; Horner, Jake A. Environmental Science & Technology, Vol. 56, Issue 20 https://doi.org/10.1021/acs.est.2c03269	journal	September 2022
Facile Metal Release from Pore-Lining Phases Enables Unique Carbonate Zonation in a Basalt Carbon Mineralization Demonstration Lahiri, Nabajit; Miller, Quin R. S.; Cao, Ruoshi Environmental Science & Technology, Vol. 57, Issue 32 https://doi.org/10.1021/acs.est.3c02075	journal	July 2023
Upscaling DAC Hubs with Wind Energy and CO₂ Mineral Storage: Considerations for Large-Scale Carbon Removal from the Atmosphere Goldberg, David S.; Nawaz, Sara; Lavin, James Environmental Science & Technology, Vol. 57, Issue 51 https://doi.org/10.1021/acs.est.3c03492	journal	December 2023
Field Validation of Supercritical CO ₂ Reactivity with Basalts McGrail, B. Peter; Schaef, Herbert T.; Spane, Frank A. Environmental Science & Technology Letters, Vol. 4, Issue 1 https://doi.org/10.1021/acs.estlett.6b00387	journal	November 2016
Strain-Induced Metastable Phase Stabilization in Ga₂O₃ Thin Films Xu, Yaobin; Park, Ji-Hyeon; Yao, Zhenpeng ACS Applied Materials & Interfaces, Vol. 11, Issue 5 https://doi.org/10.1021/acsami.8b17731	journal	January 2019
Pore-Scale Microenvironments Control Anthropogenic Carbon Mineralization Outcomes in Basalt Depp, Charles T.; Miller, Quin R. S.; Crum, Jarrod V. ACS Earth and Space Chemistry, Vol. 6, Issue 12 https://doi.org/10.1021/acsearthspacechem.2c00165	journal	November 2022
Ionic hydration enthalpies Smith, Derek W. Journal of Chemical Education, Vol. 54, Issue 9 https://doi.org/10.1021/ed054p540	journal	September 1977
Surface Chemistry and Dissolution Kinetics of Divalent Metal Carbonates Pokrovsky, O. S.; Schott, J. Environmental Science & Technology, Vol. 36, Issue 3 https://doi.org/10.1021/es010925u	journal	February 2002
Potential for carbon dioxide sequestration in flood basalts: SEQUESTRATION IN FLOOD BASALTS McGrail, B. Peter; Schaef, H. Todd; Ho, Anita M. Journal of Geophysical Research: Solid Earth, Vol. 111, Issue B12 https://doi.org/10.1029/2005JB004169	journal	December 2006
Geologically rapid aqueous mineral alteration at subfreezing temperatures in icy worlds Zandanel, Amber; Hellmann, Roland; Truche, Laurent Nature Astronomy, Vol. 6, Issue 5 https://doi.org/10.1038/s41550-022-01613-2	journal	March 2022
Phase contrast scanning transmission electron microscopy imaging of light and heavy atoms at the limit of contrast and resolution Yücelen, Emrah; Lazić, Ivan; Bosch, Eric G. T. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-20377-2	journal	February 2018
Carbon dioxide storage through mineral carbonation Snæbjörnsdóttir, Sandra Ó.; Sigfússon, Bergur; Marieni, Chiara Nature Reviews Earth & Environment, Vol. 1, Issue 2 https://doi.org/10.1038/s43017-019-0011-8	journal	January 2020
Direct air capture: process technology, techno-economic and socio-political challenges Erans, María; Sanz-Pérez, Eloy S.; Hanak, Dawid P. Energy & Environmental Science, Vol. 15, Issue 4 https://doi.org/10.1039/D1EE03523A	journal	January 2022
An experimental study on kinetically‐driven precipitation of calcium‐magnesium‐iron carbonates from solution: Implications for the low‐temperature formation of carbonates in martian meteorite Allan Hills 84001 Golden, D. C.; Ming, D. W.; Schwandt, C. S. Meteoritics & Planetary Science, Vol. 35, Issue 3 https://doi.org/10.1111/j.1945-5100.2000.tb01428.x	journal	May 2000
Direct physical evidence of dolomite recrystallization Kaczmarek, Stephen E.; Sibley, Duncan F. Sedimentology, Vol. 61, Issue 6 https://doi.org/10.1111/sed.12119	journal	May 2014
Rapid carbon mineralization for permanent disposal of anthropogenic carbon dioxide emissions Matter, J. M.; Stute, M.; Snaebjornsdottir, S. O. Science, Vol. 352, Issue 6291 https://doi.org/10.1126/science.aad8132	journal	June 2016
Net-zero emissions energy systems Davis, Steven J.; Lewis, Nathan S.; Shaner, Matthew Science, Vol. 360, Issue 6396 https://doi.org/10.1126/science.aas9793	journal	June 2018
Dissolution enables dolomite crystal growth near ambient conditions Kim, Joonsoo; Kimura, Yuki; Puchala, Brian Science, Vol. 382, Issue 6673 https://doi.org/10.1126/science.adi3690	journal	November 2023
Composition-induced microstructures in rhombohedral carbonates Barber, D. J.; Khan, M. Riaz Mineralogical Magazine, Vol. 51, Issue 359 https://doi.org/10.1180/minmag.1987.051.359.07	journal	March 1987
Synthesis, characterization, and energetics of solid solution along the dolomite-ankerite join, and implications for the stability of ordered CaFe(CO ₃ ) ₂ Chai, L.; Navrotsky, A. American Mineralogist, Vol. 81, Issue 9-10 https://doi.org/10.2138/am-1996-9-1012	journal	October 1996
On twinning and microstructures in calcite and dolomite Larsson, A. -K.; Christy, A. G. American Mineralogist, Vol. 93, Issue 1 https://doi.org/10.2138/am.2008.2520	journal	January 2008
STEM investigation of exsolution lamellae and "c" reflections in Ca-rich dolomite from the Platteville Formation, western Wisconsin Shen, Z.; Konishi, H.; Brown, P. E. American Mineralogist, Vol. 98, Issue 4 https://doi.org/10.2138/am.2013.4184	journal	March 2013
An Overview of the Status and Challenges of CO2 Storage in Minerals and Geological Formations Kelemen, Peter; Benson, Sally M.; Pilorgé, Hélène Frontiers in Climate, Vol. 1 https://doi.org/10.3389/fclim.2019.00009	journal	November 2019
Tin-bearing magnetite with nanoscale Mg-Si defects: Evidence for the early stages of mineralization in a skarn system Xu, Jing; Ciobanu, Cristiana L.; Cook, Nigel J. Frontiers in Earth Science, Vol. 10 https://doi.org/10.3389/feart.2022.994153	journal	January 2023
Diffraction Features from (101¯4) Calcite Twins Mimicking Crystallographic Ordering Németh, Péter Minerals, Vol. 11, Issue 7 https://doi.org/10.3390/min11070720	journal	July 2021

Similar Records

Exotic Carbonate Mineralization Recovered from a Deep Basalt Carbon Storage Demonstration

Journal Article · Mon Sep 26 20:00:00 EDT 2022 · Environmental Science and Technology · OSTI ID:1895590

3D Quantification of Pore Networks and Anthropogenic Carbon Mineralization in Stacked Basalt Reservoirs

Journal Article · Wed Jan 31 19:00:00 EST 2024 · Environmental Science and Technology · OSTI ID:2335501

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
58 GEOSCIENCES
environmental sciences
geochemistry

Complex carbonate phases drive geologic CO2 mineralization

Citation Formats

References (38)

Similar Records

Related Subjects

Complex carbonate phases drive geologic CO₂ mineralization