Surface Condensation of CO                         2                          onto Kaolinite

H. T. Schaef; V. A. Glezakou; A. T. Owen; S. Ramprasad; P. F. Martin; B. P. McGrail

doi:10.1021/ez400169b

Surface Condensation of CO ₂ onto Kaolinite

H. T. Schaef, V. A. Glezakou, A. T. Owen, S. Ramprasad, P. F. Martin, B. P. McGrail

Research output: Contribution to journal › Article › peer-review

64 Scopus citations

Abstract

The fundamental adsorption of CO ₂ onto poorly crystalline kaolinite (KGa-2) under conditions relevant to geologic sequestration has been investigated using a quartz crystal microbalance (QCM) and density functional theory (DFT) methods. The QCM data indicated linear adsorption of CO ₂ (0-0.3 mmol of CO ₂ /g of KGa-2) onto the kaolinite surface up through the gaseous state (0.186 g/cm ³ ). However, in the supercritical region, the extent of CO ₂ adsorption increases dramatically, reaching a peak (0.9-1.2 mmol of CO ₂ /g of KGa-2) near 0.40 g/cm ³ , before declining rapidly. DFT studies of interactions of CO ₂ with kaolinite surface models confirm that surface adsorption is favored up to ∼0.34 g/cm ³ of CO ₂ , showing distorted T-shaped CO ₂ -CO ₂ clustering, typical of supercritical CO ₂ aggregation over the surface at higher densities. Beyond this point, the adsorption energy gain for any additional CO ₂ becomes smaller than the CO ₂ interaction energy (∼0.2 eV) in the supercritical medium, resulting in the desorption of CO ₂ from the kaolinite surface.

Original language	English
Pages (from-to)	142-145
Number of pages	4
Journal	Environmental Science and Technology Letters
Volume	1
Issue number	2
DOIs	https://doi.org/10.1021/ez400169b
State	Published - Feb 11 2014
Externally published	Yes

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@article{734c1c3adca0423395e98f947627da5d,

title = " Surface Condensation of CO 2 onto Kaolinite ",

abstract = " The fundamental adsorption of CO 2 onto poorly crystalline kaolinite (KGa-2) under conditions relevant to geologic sequestration has been investigated using a quartz crystal microbalance (QCM) and density functional theory (DFT) methods. The QCM data indicated linear adsorption of CO 2 (0-0.3 mmol of CO 2 /g of KGa-2) onto the kaolinite surface up through the gaseous state (0.186 g/cm 3 ). However, in the supercritical region, the extent of CO 2 adsorption increases dramatically, reaching a peak (0.9-1.2 mmol of CO 2 /g of KGa-2) near 0.40 g/cm 3 , before declining rapidly. DFT studies of interactions of CO 2 with kaolinite surface models confirm that surface adsorption is favored up to ∼0.34 g/cm 3 of CO 2 , showing distorted T-shaped CO 2 -CO 2 clustering, typical of supercritical CO 2 aggregation over the surface at higher densities. Beyond this point, the adsorption energy gain for any additional CO 2 becomes smaller than the CO 2 interaction energy (∼0.2 eV) in the supercritical medium, resulting in the desorption of CO 2 from the kaolinite surface.",

author = "Schaef, \{H. T.\} and Glezakou, \{V. A.\} and Owen, \{A. T.\} and S. Ramprasad and Martin, \{P. F.\} and McGrail, \{B. P.\}",

note = "Publisher Copyright: {\textcopyright} 2013 American Chemical Society.",

year = "2014",

month = feb,

day = "11",

doi = "10.1021/ez400169b",

language = "English",

volume = "1",

pages = "142--145",

journal = "Environmental Science and Technology Letters",

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T1 - Surface Condensation of CO 2 onto Kaolinite

AU - Schaef, H. T.

AU - Glezakou, V. A.

AU - Owen, A. T.

AU - Ramprasad, S.

AU - Martin, P. F.

AU - McGrail, B. P.

PY - 2014/2/11

Y1 - 2014/2/11

N2 - The fundamental adsorption of CO 2 onto poorly crystalline kaolinite (KGa-2) under conditions relevant to geologic sequestration has been investigated using a quartz crystal microbalance (QCM) and density functional theory (DFT) methods. The QCM data indicated linear adsorption of CO 2 (0-0.3 mmol of CO 2 /g of KGa-2) onto the kaolinite surface up through the gaseous state (0.186 g/cm 3 ). However, in the supercritical region, the extent of CO 2 adsorption increases dramatically, reaching a peak (0.9-1.2 mmol of CO 2 /g of KGa-2) near 0.40 g/cm 3 , before declining rapidly. DFT studies of interactions of CO 2 with kaolinite surface models confirm that surface adsorption is favored up to ∼0.34 g/cm 3 of CO 2 , showing distorted T-shaped CO 2 -CO 2 clustering, typical of supercritical CO 2 aggregation over the surface at higher densities. Beyond this point, the adsorption energy gain for any additional CO 2 becomes smaller than the CO 2 interaction energy (∼0.2 eV) in the supercritical medium, resulting in the desorption of CO 2 from the kaolinite surface.

AB - The fundamental adsorption of CO 2 onto poorly crystalline kaolinite (KGa-2) under conditions relevant to geologic sequestration has been investigated using a quartz crystal microbalance (QCM) and density functional theory (DFT) methods. The QCM data indicated linear adsorption of CO 2 (0-0.3 mmol of CO 2 /g of KGa-2) onto the kaolinite surface up through the gaseous state (0.186 g/cm 3 ). However, in the supercritical region, the extent of CO 2 adsorption increases dramatically, reaching a peak (0.9-1.2 mmol of CO 2 /g of KGa-2) near 0.40 g/cm 3 , before declining rapidly. DFT studies of interactions of CO 2 with kaolinite surface models confirm that surface adsorption is favored up to ∼0.34 g/cm 3 of CO 2 , showing distorted T-shaped CO 2 -CO 2 clustering, typical of supercritical CO 2 aggregation over the surface at higher densities. Beyond this point, the adsorption energy gain for any additional CO 2 becomes smaller than the CO 2 interaction energy (∼0.2 eV) in the supercritical medium, resulting in the desorption of CO 2 from the kaolinite surface.

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U2 - 10.1021/ez400169b

DO - 10.1021/ez400169b

M3 - Article

AN - SCOPUS:84969246669

SN - 2328-8930

VL - 1

SP - 142

EP - 145

JO - Environmental Science and Technology Letters

JF - Environmental Science and Technology Letters

IS - 2

ER -

Surface Condensation of CO ₂ onto Kaolinite

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