A reactive-transport model for examining tectonic and climatic controls on chemical weathering and atmospheric CO2 consumption in granitic regolith

We developed a 1D reactive-transport model for examining how tectonic and climatic parameters, namely uplift rate, water seepage velocity, and temperature, control chemical weathering and atmospheric CO2 consumption rates during regolith development. The model consists of mass-conservation equations describing how mineral and solute concentrations change temporally and spatially (vertically) during weathering of granite containing 30% plagioclase (An(20)) and up to 3% accessory calcite. The equations are coupled by volumetric weathering rates, which depend on mineral abundances, intrinsic dissolution rate constants, and surface areas as well as the departure of pore water from thermodynamic equilibrium. We numerically solve a non-steady-state, non-dimensional version of the model. By eliminating the need to prescribe regolith thickness, non-dimensionalization introduces two key scaling parameters that drive variations in the model results: the rock residence time T-r, the time for rock to travel upward through the model domain) and the water residence time (T-w, the time for water to travel downward through the model domain). We use the model to examine fundamental properties of chemical weathering, especially reaction front propagation, with the primary aim of characterizing weathering regimes and identifying factors that maximize the dissolution of plagioclase because only silicate weathering regulates atmospheric CO2 levels over geological timescales. Weathering regimes are commonly classified as transport (or supply)-limited versus weathering (or kinetically)limited, but as outgrowths of geomorphology, these terms primarily refer to the role of tr in regulating regolith thickness. Our findings suggest that the paradigm should be expanded to include kinetic controls determined by T-w. Both regimes can experience far-from-and near-equilibrium mineral dissolution. However, transport-limited regimes generally have lower T-w/T-r ratios compared to kinetically-limited regimes. Under transport limitation, thick to thin reaction fronts propagate downward indefinitely yielding extensive mineral depletion, deeply weathered regolith, and high ratios of silicate-to-carbonate weathering. Under kinetic limitation, thin to non-existent reaction fronts evolve to steady-state yielding minimal mineral depletion, no regolith development, and low ratios of silicate-to-carbonate weathering. Kinetically-limited regimes typifying tectonically active mountain ranges have low long-term atmospheric CO2 consumption rates. Transport-limited regimes typifying tectonically stable cratons also have low long-term atmospheric CO2 consumption rates, but because much of the Earth's surface is transport-limited, we infer that such environments have the greatest impact on the global atmospheric CO2 consumption flux. The model output leads us to hypothesize that the maximum contribution should occur for extensive regions of silicate bedrock consolidated in warm, wet climates because the combination of tectonic stability, high temperatures, and rapid seepage velocities accelerates reaction front propagation, facilitates calcite depletion, and sustains deep regolith development over long timescales. Our findings point to the importance of internal climate feedbacks for stabilizing long-term atmospheric CO2 levels. (C) 2013 Elsevier B. V. All rights reserved.