TY - JOUR
T1 - Porosity and surface area evolution during weathering of two igneous rocks
AU - Navarre-Sitchler, Alexis K.
AU - Cole, David R.
AU - Rother, Gernot
AU - Jin, Lixin
AU - Buss, Heather L.
AU - Brantley, Susan L.
N1 - Funding Information:
S.L.B. acknowledges NSF CHE-0431328 and DOE DE-FG02-05ER15675 ; D.R.C. acknowledges support from the Basic Energy Sciences Energy Frontier Research Center “Nanoscale Control of Geologic CO 2 ”. G.R. acknowledges support from the Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy. Oak Ridge National Laboratory is managed by UT-Battelle, LLC for the U.S. Department of Energy under Contract DE-AC05-00OR22725. D. Mildner, A. Jackson and the National Institute of Standards and Technology, U.S. Department of Commerce, are acknowledged for neutron beam support and facilities. Anonymous reviewers are acknowledged for their thoughtful and very helpful comments on an earlier version of this manuscript. H. Buss acknowledges support from the Luquillo Critical Zone Observatory and funding from NSF EAR-0722476 to F. Scatena (Univ. of Pennsylvania). We thank Jorgen Rosenqvist for performing BET analysis on the basaltic andesite samples at Oak Ridge National Laboratory.
PY - 2013/5/5
Y1 - 2013/5/5
N2 - During weathering, rocks release nutrients and store water vital for growth of microbial and plant life. Thus, the growth of porosity as weathering advances into bedrock is a life-sustaining process for terrestrial ecosystems. Here, we use small-angle and ultra small-angle neutron scattering to show how porosity develops during initial weathering under tropical conditions of two igneous rock compositions, basaltic andesite and quartz diorite. The quartz diorite weathers spheroidally while the basaltic andesite does not. The weathering advance rates of the two systems also differ, perhaps due to this difference in mechanism, from 0.24 to 100mmkyr-1, respectively. The scattering data document how surfaces inside the feldspar-dominated rocks change as weathering advances into the protolith. In the unaltered rocks, neutrons scatter from two types of features whose dimensions vary from 6nm to 40μm: pores and bumps on pore-grain surfaces. These features result in scattering data for both unaltered rocks that document multi-fractal behavior: scattering is best described by a mass fractal dimension (Dm) and a surface fractal dimension (Ds) for features of length scales greater than and less than ∼1μm, respectively. In the basaltic andesite, Dm is approximately 2.9 and Ds is approximately 2.7. The mechanism of solute transport during weathering of this rock is diffusion. Porosity and surface area increase from ∼1.5% to 8.5% and 3 to 23m2g-1 respectively in a relatively consistent trend across the mm-thick plagioclase reaction front. Across this front, both fractal dimensions decrease, consistent with development of a more monodisperse pore network with smoother pore surfaces. Both changes are consistent largely with increasing connectivity of pores without significant surface roughening, as expected for transport-limited weathering. In contrast, porosity and surface area increase from 1.3% to 9.5% and 1.5 to 13m2g-1 respectively across a many cm-thick reaction front in the spheroidally weathering quartz diorite. In that rock, Dm is approximately 2.8 and Ds is approximately 2.5 prior to weathering. These two fractals transform during weathering to multiple surface fractals as micro-cracking reduces the size of diffusion-limited subzones of the matrix. Across the reaction front of plagioclase in the quartz diorite, the specific surface area and porosity change very little until the point where the rock disaggregates into saprolite.The different patterns in porosity development of the two rocks are attributed to advective infiltration plus diffusion in the rock that spheroidally fractures versus diffusion-only in the rock that does not. Fracturing apparently diminishes the size of the diffusion-limited parts of the spheroidally weathering rock system to promote infiltration of meteoric fluids, therefore explaining the faster weathering advance rate into that rock.
AB - During weathering, rocks release nutrients and store water vital for growth of microbial and plant life. Thus, the growth of porosity as weathering advances into bedrock is a life-sustaining process for terrestrial ecosystems. Here, we use small-angle and ultra small-angle neutron scattering to show how porosity develops during initial weathering under tropical conditions of two igneous rock compositions, basaltic andesite and quartz diorite. The quartz diorite weathers spheroidally while the basaltic andesite does not. The weathering advance rates of the two systems also differ, perhaps due to this difference in mechanism, from 0.24 to 100mmkyr-1, respectively. The scattering data document how surfaces inside the feldspar-dominated rocks change as weathering advances into the protolith. In the unaltered rocks, neutrons scatter from two types of features whose dimensions vary from 6nm to 40μm: pores and bumps on pore-grain surfaces. These features result in scattering data for both unaltered rocks that document multi-fractal behavior: scattering is best described by a mass fractal dimension (Dm) and a surface fractal dimension (Ds) for features of length scales greater than and less than ∼1μm, respectively. In the basaltic andesite, Dm is approximately 2.9 and Ds is approximately 2.7. The mechanism of solute transport during weathering of this rock is diffusion. Porosity and surface area increase from ∼1.5% to 8.5% and 3 to 23m2g-1 respectively in a relatively consistent trend across the mm-thick plagioclase reaction front. Across this front, both fractal dimensions decrease, consistent with development of a more monodisperse pore network with smoother pore surfaces. Both changes are consistent largely with increasing connectivity of pores without significant surface roughening, as expected for transport-limited weathering. In contrast, porosity and surface area increase from 1.3% to 9.5% and 1.5 to 13m2g-1 respectively across a many cm-thick reaction front in the spheroidally weathering quartz diorite. In that rock, Dm is approximately 2.8 and Ds is approximately 2.5 prior to weathering. These two fractals transform during weathering to multiple surface fractals as micro-cracking reduces the size of diffusion-limited subzones of the matrix. Across the reaction front of plagioclase in the quartz diorite, the specific surface area and porosity change very little until the point where the rock disaggregates into saprolite.The different patterns in porosity development of the two rocks are attributed to advective infiltration plus diffusion in the rock that spheroidally fractures versus diffusion-only in the rock that does not. Fracturing apparently diminishes the size of the diffusion-limited parts of the spheroidally weathering rock system to promote infiltration of meteoric fluids, therefore explaining the faster weathering advance rate into that rock.
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U2 - 10.1016/j.gca.2013.02.012
DO - 10.1016/j.gca.2013.02.012
M3 - Article
AN - SCOPUS:84875597150
SN - 0016-7037
VL - 109
SP - 400
EP - 413
JO - Geochimica et Cosmochimica Acta
JF - Geochimica et Cosmochimica Acta
ER -