Coupled feldspar dissolution and secondary mineral precipitation in batch systems: 6. Labradorite dissolution, calcite growth, and clay precipitation at 60&nbsp;°C and pH 8.2–8.4

Chen, Mingkun; Gong, Lei; Schott, Jacques; Lu, Peng; Chen, Kaiyun; Yuan, Honglin; Sun, Jian; Chen, Si Athena; Apps, John; Zhu, Chen

doi:10.1016/j.gca.2024.11.030

Coupled feldspar dissolution and secondary mineral precipitation in batch systems: 6. Labradorite dissolution, calcite growth, and clay precipitation at 60 °C and pH 8.2–8.4

Journal Article · Sun Dec 01 23:00:00 EST 2024 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2024.11.030· OSTI ID:2538568

^[1]; Gong, Lei ^[2]; Schott, Jacques ^[3]; ^[4]; Chen, Kaiyun ^[5]; Yuan, Honglin ^[5]; ^[6]; Chen, Si Athena ^[7]; Apps, John ^[8]; ^[2]

Indiana University, Bloomington, IN (United States); Dalian University of Technology (China)
Indiana University, Bloomington, IN (United States)
Centre National de la Recherche Scientifique (CNRS), Toulouse (France); Université Toulouse 3-Paul Sabatier (UPS) (France); Observatoire Midi-Pyrénées (OMP), Toulouse (France); Géosciences Environnement Toulouse (France)
Indiana University, Bloomington, IN (United States); Saudi Aramco, Dhahran (Saudi Arabia). EXPEC Advanced Research Center
Northwest University, Xi’an (China)
Chinese Academy of Geological Sciences, Beijing (China)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Here, we conducted experiments on concurrent labradorite dissolution, calcite precipitation, and clay precipitation in batch reactor systems and tracked reaction processes using multiple isotope tracers. Labradorite was chosen for its role as a major and reactive component in basalt; the experiments thus directly impact our understanding of CO₂ storage in basalt aquifers and enhanced rock weathering. We doped initial solutions with ²⁹Si, ⁴³Ca, and Ca¹³CO₃(s). Experiments were conducted at 60 °C and pH ~ 8.3 for up to 840 h, with isotope ratios in the experimental aqueous solutions measured using MC-ICP-MS. Unidirectional rates of labradorite dissolution near equilibrium were approximately two orders of magnitude slower than far-from-equilibrium rates reported in the literature. Calcite growth occurred near equilibrium and the rates were limited by the labradorite dissolution rates. In the steady state phase, the interplay of these three heterogeneous reactions—labradorite dissolution, calcite growth, and clay precipitation—results in a coupled system that approaches a near-equilibrium state. The system does not reach true equilibrium because labradorite continues to dissolve, albeit at a much slower rate near equilibrium. The overall reaction can be approximated as, Na_0.4Ca_0.6Al_1.6Si_2.4O₈ + 0.6HCO₃^- + 1·.7H₂O + 0.4H⁺ → 0.4Na⁺ + 0.6CaCO_3(s) + 0.5Al₂Si₂O₅(OH)_4(s) + 0.6Al(OH)₄^- + 1.4SiO₂^o(aq). The experimental results show that using short-term far-from-equilibrium rate constants would lead to an overestimation of feldspar weathering rates at the Earth’s surface (e.g., basalt weathering and enhanced rock weathering) and CO₂ mineralization in basalt aquifers.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NS)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2538568

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Vol. 390; ISSN 0016-7037

Publisher:: Elsevier; The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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