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Title: Thickness measurements of nanoscale brine films on silica surfaces under geologic CO 2 sequestration conditions using synchrotron X-ray fluorescence

Abstract

In reservoirs used for geologic CO2 sequestration, brine films remaining on mineral surfaces can influence flow, diffusion, and reactions. We have examined how the capillary (disjoining) potential influences the thickness of a KCsI2 brine film on both smooth and rough SiO2 surfaces [root mean square roughness (Rrms), 1.6 and 330 nm, respectively], under confinement with supercritical (sc) CO2. The thicknesses of brine films coating interior surfaces of SiO2 windows in a high-pressure cell were determined through synchrotron X-ray fluorescence of two tracer ions (I- and Cs+) at 7.8 MPa and 40°C (representative of conditions at about 0.78 km below the land surface), with scCO2 as the immiscible confining fluid. The measured area-averaged film thicknesses on the 330 nm Rrms silica surface ranged from 265 to 249 nm for capillary potentials measured within a narrow range from 0.18 to 3.7 kPa. Over this same range of potentials, film thicknesses measured on the smooth (1.6 nm Rrms) silica surface were about 2 nm, although equilibrium does not seem to have been achieved. The measured average brine film thicknesses were critically controlled by surface roughness, with very weak variation in response to the fairly narrow range of tested capillary potentials.

Authors:
 [1];  [2];  [2];  [3];  [4];  [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Stanford Univ., Stanford, CA (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Univ. of Chicago, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1508045
Report Number(s):
DOE-UCHICAGO-14466-9
Journal ID: ISSN 0043-1397
Grant/Contract Number:  
FG02-94ER14466
Resource Type:
Accepted Manuscript
Journal Name:
Water Resources Research
Additional Journal Information:
Journal Volume: 48; Journal Issue: 9; Journal ID: ISSN 0043-1397
Publisher:
American Geophysical Union (AGU)
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; CO2 sequestration; brine film; capillary pressure; roughness; synchrotron X‐rays

Citation Formats

Kim, Tae Wook, Tokunaga, Tetsu K., Shuman, Derek B., Sutton, Stephen R., Newville, Matt, and Lanzirotti, Antonio. Thickness measurements of nanoscale brine films on silica surfaces under geologic CO 2 sequestration conditions using synchrotron X-ray fluorescence. United States: N. p., 2012. Web. doi:10.1029/2012WR012200.
Kim, Tae Wook, Tokunaga, Tetsu K., Shuman, Derek B., Sutton, Stephen R., Newville, Matt, & Lanzirotti, Antonio. Thickness measurements of nanoscale brine films on silica surfaces under geologic CO 2 sequestration conditions using synchrotron X-ray fluorescence. United States. https://doi.org/10.1029/2012WR012200
Kim, Tae Wook, Tokunaga, Tetsu K., Shuman, Derek B., Sutton, Stephen R., Newville, Matt, and Lanzirotti, Antonio. Sat . "Thickness measurements of nanoscale brine films on silica surfaces under geologic CO 2 sequestration conditions using synchrotron X-ray fluorescence". United States. https://doi.org/10.1029/2012WR012200. https://www.osti.gov/servlets/purl/1508045.
@article{osti_1508045,
title = {Thickness measurements of nanoscale brine films on silica surfaces under geologic CO 2 sequestration conditions using synchrotron X-ray fluorescence},
author = {Kim, Tae Wook and Tokunaga, Tetsu K. and Shuman, Derek B. and Sutton, Stephen R. and Newville, Matt and Lanzirotti, Antonio},
abstractNote = {In reservoirs used for geologic CO2 sequestration, brine films remaining on mineral surfaces can influence flow, diffusion, and reactions. We have examined how the capillary (disjoining) potential influences the thickness of a KCsI2 brine film on both smooth and rough SiO2 surfaces [root mean square roughness (Rrms), 1.6 and 330 nm, respectively], under confinement with supercritical (sc) CO2. The thicknesses of brine films coating interior surfaces of SiO2 windows in a high-pressure cell were determined through synchrotron X-ray fluorescence of two tracer ions (I- and Cs+) at 7.8 MPa and 40°C (representative of conditions at about 0.78 km below the land surface), with scCO2 as the immiscible confining fluid. The measured area-averaged film thicknesses on the 330 nm Rrms silica surface ranged from 265 to 249 nm for capillary potentials measured within a narrow range from 0.18 to 3.7 kPa. Over this same range of potentials, film thicknesses measured on the smooth (1.6 nm Rrms) silica surface were about 2 nm, although equilibrium does not seem to have been achieved. The measured average brine film thicknesses were critically controlled by surface roughness, with very weak variation in response to the fairly narrow range of tested capillary potentials.},
doi = {10.1029/2012WR012200},
journal = {Water Resources Research},
number = 9,
volume = 48,
place = {United States},
year = {Sat Sep 29 00:00:00 EDT 2012},
month = {Sat Sep 29 00:00:00 EDT 2012}
}

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