Oxidation and Associated Pore Structure Modification During Experimental Alteration of Granite

Journal Article · 01 January 2021 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2020.08.016· OSTI ID:1713196

Anovitz, Lawrence M. ^[1]; Cheshire, Michael ^[1]; Hermann, Raphael ^[1]; Gu, Xin ^[2]; Sheets, Julia ^[3]; Brantley, Susan L. ^[2]; Cole, David R. ^[4]; Ilton, Eugene S. ^[5]; Mildner, David ^[6]; Gagnon, Cedric ^[6]; Allard, Lawrence F. ^[1]; Littrell, Kenneth C. ^[1]

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1. Oak Ridge National Laboratory
2. Pennsylvania State University
3. Ohio State University
4. OHIO STATE UNIVERSITY
5. BATTELLE (PACIFIC NW LAB)
6. NIST Center for Neutron Research

Weathering plays a crucial role in a number of environmental processes, and the microstructure and evolution of multi-scale pore space is a critically important factor in the weathering of geological formations. In igneous rocks the infiltration of meteoric water into initially relatively dry material can cause the rock to begin to disaggregate, increasing porosity and surface area, and allowing further disaggregation and weathering to occur. These processes, in turn, allow biota to colonize the rock, further enhancing the weathering rate. In some igneous rocks this may be driven by oxidation of primary minerals. One such mineral, biotite, has been repeatedly mentioned as a cause of cracking during oxidation. However, the scale-dependence of the processes by which this occurs are poorly understood. We cannot, therefore, accurately extrapolate laboratory reaction rates to the field in predictive numerical models. In order to better understand the effects of oxidation and test the hypothesis that fracture and disaggregation are initiated by swelling of oxidizing biotites, we reacted granite cores in a selenic acid-rich aqueous solution at 200°C for up to 438 days. Elevated temperatures and selenic acid were used to provide relatively fast reaction rates and highly oxidizing conditions in sealed reaction vessels. These experiments were analyzed using a combination of imaging, X-ray diffraction, Mössbauer spectroscopy, and small- and ultra-small angle neutron scattering to interrogate porosity and microfracture formation. The experimental results show little observable biotite swelling, but significant transport and growth of iron oxides and/or clays along grain boundaries throughout the sample. Significant increases in porosity were also observed at the sample rim, likely associated with feldspar alteration. Fractures and transport were observed throughout the core, suggesting that stresses due to crystallization pressures caused by the growing iron phases may be the initiating factors in granite weathering, possibly followed by biotite swelling after sufficient permeability is achieved.

• Research Organization: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
• Sponsoring Organization: USDOE
• DOE Contract Number: AC05-76RL01830
• OSTI ID: 1713196
• Report Number(s): PNNL-SA-156276
• Journal Information: Geochimica et Cosmochimica Acta, Vol. 292
• Country of Publication: United States
• Language: English