Influence of CO2 on Nanoconfined Water in a Clay Mineral
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Influence of CO2 on Nanoconfined Water in a Clay Mineral. / Hunvik, Kristoffer W. Bo; Lima, Rodrigo Jose da Silva; Kirch, Alexsandro; Loch, Patrick; Roren, Paul Monceyron; Petersen, Martin Hoffmann; Rudic, Svemir; Sakai, Victoria Garcia; Knudsen, Kenneth Dahl; Instituto, Caetano Rodrigues Miranda Materiais; Breu, Josef; Fossum, Jon Otto; Bordallo, Heloisa N.
In: Journal of Physical Chemistry C, Vol. 126, No. 40, 13.10.2022, p. 17243-17254.Research output: Contribution to journal › Journal article › Research › peer-review
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TY - JOUR
T1 - Influence of CO2 on Nanoconfined Water in a Clay Mineral
AU - Hunvik, Kristoffer W. Bo
AU - Lima, Rodrigo Jose da Silva
AU - Kirch, Alexsandro
AU - Loch, Patrick
AU - Roren, Paul Monceyron
AU - Petersen, Martin Hoffmann
AU - Rudic, Svemir
AU - Sakai, Victoria Garcia
AU - Knudsen, Kenneth Dahl
AU - Instituto, Caetano Rodrigues Miranda Materiais
AU - Breu, Josef
AU - Fossum, Jon Otto
AU - Bordallo, Heloisa N.
PY - 2022/10/13
Y1 - 2022/10/13
N2 - Developing new technologies for carbon sequestra-tion and long-term carbon storage is important. Clay minerals are interesting in this context as they are low-cost, naturally abundant, can adsorb considerable amounts of CO2, and are present in storage sites for anthropogenic carbon. Here, to better understand the intercalation mechanisms of CO2 in dehydrated and hydrated synthetic Na-fluorohectorite clay, we have combined powder X-ray diffraction, inelastic and quasi-elastic neutron scattering, and density functional theory calculations. For dehydrated Na-fluorohectorite, we observe no crystalline swelling or spectroscopic changes in response to CO2, whereas for the hydrated case, damping of the librational modes related to the intercalated water was clearly observed. These findings suggest the formation of a more disordered water coordination in the interlayer associated with highly confined water molecules. From the simulations, we conclude that intercalated water molecules decrease the layer-layer cohesion energy and create physical space for CO2 intercalation. Furthermore, we confirm that interlayer confinement reduces the Na+ hydration number when compared to that in bulk aqueous water, which may allow for proton transfer and hydroxide formation followed by CO2 adsorption in the form of carbonates. The experimental results are discussed in the context of previous and present observations on, a similar smectite, Ni-fluorohectorite, for which it is established that CO2 attaches to the edge of nickel hydroxide islands present in the interlayer.
AB - Developing new technologies for carbon sequestra-tion and long-term carbon storage is important. Clay minerals are interesting in this context as they are low-cost, naturally abundant, can adsorb considerable amounts of CO2, and are present in storage sites for anthropogenic carbon. Here, to better understand the intercalation mechanisms of CO2 in dehydrated and hydrated synthetic Na-fluorohectorite clay, we have combined powder X-ray diffraction, inelastic and quasi-elastic neutron scattering, and density functional theory calculations. For dehydrated Na-fluorohectorite, we observe no crystalline swelling or spectroscopic changes in response to CO2, whereas for the hydrated case, damping of the librational modes related to the intercalated water was clearly observed. These findings suggest the formation of a more disordered water coordination in the interlayer associated with highly confined water molecules. From the simulations, we conclude that intercalated water molecules decrease the layer-layer cohesion energy and create physical space for CO2 intercalation. Furthermore, we confirm that interlayer confinement reduces the Na+ hydration number when compared to that in bulk aqueous water, which may allow for proton transfer and hydroxide formation followed by CO2 adsorption in the form of carbonates. The experimental results are discussed in the context of previous and present observations on, a similar smectite, Ni-fluorohectorite, for which it is established that CO2 attaches to the edge of nickel hydroxide islands present in the interlayer.
KW - INELASTIC NEUTRON-SCATTERING
KW - CARBON-DIOXIDE
KW - X-RAY
KW - HYDRATION PROPERTIES
KW - INTERCALATED WATER
KW - MOLECULAR-DYNAMICS
KW - SUPERCRITICAL CO2
KW - SMECTITE CLAYS
KW - ADSORPTION
KW - INTERLAYER
U2 - 10.1021/acs.jpcc.2c03310
DO - 10.1021/acs.jpcc.2c03310
M3 - Journal article
VL - 126
SP - 17243
EP - 17254
JO - The Journal of Physical Chemistry Part C
JF - The Journal of Physical Chemistry Part C
SN - 1932-7447
IS - 40
ER -
ID: 324368406