当前位置: X-MOL 学术Transp Porous Media › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Statistical Characterization of Heterogeneous Dissolution Rates of Calcite from In situ and Real-Time AFM Imaging
Transport in Porous Media ( IF 2.7 ) Pub Date : 2021-06-20 , DOI: 10.1007/s11242-021-01624-z
Martina Siena , Gianlorenzo Bussetti , Chiara Recalcati , Monica Riva , Lamberto Duò , Alberto Guadagnini

Abstract

The evolution of the surface topography of a calcite crystal subject to dissolution is documented through in situ real-time imaging obtained via atomic force microscopy (AFM). The dissolution process takes place by exposing the crystal surface to deionized water. AFM data allow detection of nucleation and expansion of mono- and multilayer rhombic etch pits and are employed to estimate the spreading rate of these structures. Spatially heterogeneous distributions of local dissolution rate are evaluated from the difference between topographic measurements taken at prescribed time intervals. We rest on a stochastic framework of analysis viewing the dissolution rate as a generalized sub-Gaussian (GSG) spatially correlated random process. Our analysis yields: (i) a quantitative assessment of the temporal evolution of the statistics of the dissolution rates as well as their spatial increments; (ii) a characterization of the degree of spatial correlation of dissolution rates and of the way this is linked to the various mechanisms involved in the dissolution process and highlighted through the experimental evidences. Our results indicate that the parameters driving the statistics of the GSG distribution and the spreading rate of the multilayer pits display a similar trend in time, thus suggesting that the evolution of these structures imprints the statistical features of local dissolution rates.

Article Highlights

  • We investigate dynamics of dissolution patterns on a calcite crystal in contact with deionized water via AFM imaging

  • Temporal behavior of parameters of our statistical model is consistent with surface pattern evolution

  • A nested model for the spatial correlation of rates embeds multiple mechanisms driving dissolution rate.



中文翻译:

来自原位和实时 AFM 成像的方解石异质溶解率的统计表征

摘要

通过原子力显微镜 (AFM) 获得的原位实时成像记录了易于溶解的方解石晶体表面形貌的演变。溶解过程是通过将晶体表面暴露于去离子水而发生的。AFM 数据允许检测单层和多层菱形蚀刻坑的成核和扩展,并用于估计这些结构的扩散率。局部溶解速率的空间异质分布是根据在规定时间间隔内进行的地形测量之间的差异来评估的。我们基于一个随机分析框架,将溶出率视为广义亚高斯 (GSG) 空间相关随机过程。我们的分析得出:(i) 对溶解速率统计数据的时间演变及其空间增量的定量评估;(ii) 溶解速率的空间相关程度的特征以及它与溶解过程中涉及的各种机制的联系方式,并通过实验证据突出显示。我们的结果表明,驱动 GSG 分布统计和多层凹坑扩散速率的参数随时间显示出相似的趋势,因此表明这些结构的演变印记了局部溶解速率的统计特征。(ii) 溶解速率的空间相关程度的特征以及它与溶解过程中涉及的各种机制的联系方式,并通过实验证据突出显示。我们的结果表明,驱动 GSG 分布统计和多层凹坑扩散速率的参数随时间显示出相似的趋势,因此表明这些结构的演变印记了局部溶解速率的统计特征。(ii) 溶解速率的空间相关程度的特征以及它与溶解过程中涉及的各种机制的联系方式,并通过实验证据突出显示。我们的结果表明,驱动 GSG 分布统计和多层凹坑扩散速率的参数随时间显示出相似的趋势,因此表明这些结构的演变印记了局部溶解速率的统计特征。

文章亮点

  • 我们通过 AFM 成像研究了与去离子水接触的方解石晶体的溶解模式动力学

  • 我们的统计模型参数的时间行为与表面图案演变一致

  • 速率空间相关性的嵌套模型嵌入了多种驱动溶出速率的机制。

更新日期:2021-06-20
down
wechat
bug