期刊
APPLIED SURFACE SCIENCE
卷 549, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apsusc.2021.149317
关键词
Olivine dissolution; Rate variation; Gibbs free energy; VSI; AFM; Raman
类别
资金
- National Key R&D Program of China [2017YFB0309902]
- National Natural Science Foundation of China [51602148, 52072171]
- Joint Funds of the National Natural Science Foundation of China [U1806222]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- China Scholarship Council [201808320374]
- German Ministry for Education and Research (BMBF) [03G0871A]
- German Research Foundation (DFG) [INST 144/378-1, INST 144/388-1]
- Jiangsu National Synergetic Innovation Centre for Advanced Materials (SICAM)
This study investigates the dissolution process of olivine materials on the (010) surface in acidic solutions, revealing the temporal and spatial variation of dissolution rates and indicating that surface reactivity is better defined by rate ranges under far from equilibrium conditions.
The surface reaction of olivine materials is critical for their extensive applications in the global cycle of elements, future CO2 sequestration and fuel production. Here, we investigate a pristine (010) surface dissolved in flow-through cells with acidic solutions at surface control regime. The multiscale surface topography changes during dissolution are firstly measured by a combination of ex-situ vertical scanning interferometry and in-situ atomic force microscopy (AFM). The deduced dissolution rate maps and rate spectra from surface topography vary temporally and spatially, wherein the average rate is higher at initial stages and reaches to a constant value, about 6.6 +/- 1 x 10(-8) mol m(-2) s(-1), after 100 h reaction accompanied with the formation of crystallographically controlled pits. Furthermore, in-situ AFM shows that the average height of steps on the pit walls is equal to 1/2b and Raman spectra prevails that the (010) surface is favorably dissolved layer by layer at Mg2 glide plane with SiO44- distortion. This work reveals that at far from equilibrium conditions with constant Gibbs free energy, surface reactivity is better defined by rate ranges rather than a single mean rate. This superior method is powerful to quantify surface reaction variabilities in multiscale range and understand the geochemical cycles.
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