Recent numerical investigations revealed that the heterogeneity of the dissolution rate observed in numerous experiments cannot be explained by fluid transport effects. This heterogeneity is attributed to intrinsic surface reactivity. Therefore, reactive transport models (RTM) require parameterization of the surface reactivity for accurate predictions. For this purpose, a nanotopographic parametrization based on surface slope has been recently suggested. In this study, we utilize and improve this parametrization for RTMs of pore-scale systems, from the crystal surface to the single crystal geometry, going beyond the previous reactivity parametrization. 2D and 3D RTMs were developed using COMSOL Multiphysics for calcite systems based on experimental measurements. We compared the results between classically parameterized RTMs, RTMs with new slope parameterization, and experimental data. The effect of flow on dissolution under conditions far-from-equilibrium is found to be negligible, highlighting the importance of surface reactivity in the dissolution reaction. For the first time, the new slope factor was able to accurately reproduce the experimental results on a crystal surface with large field-of-view, large height variability of the topography, and over a long-term reaction period. The new parameterization had greatly improved sensitivity for intermediate reactivity ranges compared to the previous parameterization. A 3D model is used to present the general applicability of the parameterization for use in realistic geometric data sets. Thus, we also show that neglecting surface reactivity in an RTM leads to incorrect predictions regarding the porosity, pore geometry, and surface topography of the system. Our new slope factor can successfully serve as a first-order proxy for the distribution of surface reactivity in 3D pore-scale rock systems. The description of surface reactivity is crucial for accurate long-term modeling of natural rock systems.

最近的数值研究表明，在许多实验中观察到的溶解速率的异质性不能用流体传输效应来解释。这种异质性归因于内在的表面反应性。因此，反应性传输模型 (RTM) 需要对表面反应性进行参数化以进行准确预测。为此，最近提出了基于表面斜率的纳米形貌参数化。在这项研究中，我们利用和改进了孔隙尺度系统 RTM 的这种参数化，从晶体表面到单晶几何形状，超越了之前的反应性参数化。基于实验测量，使用 COMSOL Multiphysics 为方解石系统开发了 2D 和 3D RTM。我们比较了经典参数化 RTM 之间的结果，具有新斜率参数化和实验数据的 RTM。发现在远离平衡的条件下流动对溶解的影响可以忽略不计，这突出了表面反应性在溶解反应中的重要性。新的斜率因子首次能够在具有大视场、地形高度可变性和长期反应周期的晶体表面上准确再现实验结果。与之前的参数化相比，新的参数化极大地提高了中间反应范围的灵敏度。3D 模型用于展示参数化在现实几何数据集中的一般适用性。因此，我们还表明，忽略 RTM 中的表面反应性会导致对孔隙度、孔隙几何形状、和系统的表面形貌。我们的新坡度因子可以成功地作为 3D 孔隙尺度岩石系统中表面反应性分布的一级代理。表面反应性的描述对于天然岩石系统的准确长期建模至关重要。