Carbon Capture by Metal Oxides: Unleashing the Potential of the (111) Facet

Greg A. Mutch, Sarah Shulda, Alan J. McCue, Martin J. Menart, Cristian V. Ciobanu, Chilan Ngo, James A. Anderson, Ryan M. Richards, David Vega-Maza

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Abstract

Solid metal oxides for carbon capture exhibit reduced adsorption capacity following high-temperature exposure, due to surface area reduction by sintering. Furthermore, only low-coordinate corner/edge sites on the thermodynamically stable (100) facet display favorable binding toward CO2, providing inherently low capacity. The (111) facet, however, exhibits a high concentration of low-coordinate sites. In this work, MgO(111) nanosheets displayed high capacity for CO2, as well as a ∼65% increase in capacity despite a ∼30% reduction in surface area following sintering (0.77 mmol g–1 @ 227 m2 g–1 vs 1.28 mmol g–1 @ 154 m2 g–1). These results, unique to MgO(111), suggest intrinsic differences in the effects of sintering on basic site retention. Spectroscopic and computational investigations provided a new structure–activity insight: the importance of high-temperature activation to unleash the capacity of the polar (111) facet of MgO. In summary, we present the first example of a faceted sorbent for carbon capture and challenge the assumption that sintering is necessarily a negative process; here we leverage high-temperature conditions for facet-dependent surface activation.
Original languageEnglish
Pages (from-to)4736-4742
Number of pages7
JournalJournal of the American Chemical Society
Volume140
Issue number13
Early online date19 Mar 2018
DOIs
Publication statusPublished - 4 Apr 2018

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Carbon capture
Oxides
Sintering
Carbon
Metals
Temperature
Chemical activation
Adsorption
Nanosheets
Sorbents

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Carbon Capture by Metal Oxides : Unleashing the Potential of the (111) Facet. / Mutch, Greg A.; Shulda, Sarah; McCue, Alan J.; Menart, Martin J.; Ciobanu, Cristian V.; Ngo, Chilan; Anderson, James A.; Richards, Ryan M.; Vega-Maza, David.

In: Journal of the American Chemical Society, Vol. 140, No. 13, 04.04.2018, p. 4736-4742.

Research output: Contribution to journalArticle

Mutch, GA, Shulda, S, McCue, AJ, Menart, MJ, Ciobanu, CV, Ngo, C, Anderson, JA, Richards, RM & Vega-Maza, D 2018, 'Carbon Capture by Metal Oxides: Unleashing the Potential of the (111) Facet' Journal of the American Chemical Society, vol. 140, no. 13, pp. 4736-4742. https://doi.org/10.1021/jacs.8b01845
Mutch, Greg A. ; Shulda, Sarah ; McCue, Alan J. ; Menart, Martin J. ; Ciobanu, Cristian V. ; Ngo, Chilan ; Anderson, James A. ; Richards, Ryan M. ; Vega-Maza, David. / Carbon Capture by Metal Oxides : Unleashing the Potential of the (111) Facet. In: Journal of the American Chemical Society. 2018 ; Vol. 140, No. 13. pp. 4736-4742.
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abstract = "Solid metal oxides for carbon capture exhibit reduced adsorption capacity following high-temperature exposure, due to surface area reduction by sintering. Furthermore, only low-coordinate corner/edge sites on the thermodynamically stable (100) facet display favorable binding toward CO2, providing inherently low capacity. The (111) facet, however, exhibits a high concentration of low-coordinate sites. In this work, MgO(111) nanosheets displayed high capacity for CO2, as well as a ∼65{\%} increase in capacity despite a ∼30{\%} reduction in surface area following sintering (0.77 mmol g–1 @ 227 m2 g–1 vs 1.28 mmol g–1 @ 154 m2 g–1). These results, unique to MgO(111), suggest intrinsic differences in the effects of sintering on basic site retention. Spectroscopic and computational investigations provided a new structure–activity insight: the importance of high-temperature activation to unleash the capacity of the polar (111) facet of MgO. In summary, we present the first example of a faceted sorbent for carbon capture and challenge the assumption that sintering is necessarily a negative process; here we leverage high-temperature conditions for facet-dependent surface activation.",
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AU - Mutch, Greg A.

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AU - Ciobanu, Cristian V.

AU - Ngo, Chilan

AU - Anderson, James A.

AU - Richards, Ryan M.

AU - Vega-Maza, David

N1 - This work was supported by the Engineering and Physical Sciences Research Council (EPSRC) via a Doctoral Training Grant for G.A.M. (EP/K0502960/1) and a Doctoral Prize Fellowship (EP/M50791X/1). Dedicated to the memory of Kenneth J. Klabunde. Supporting Information. Synthesis procedure, experimental methods, computational methods, transmission microscopy images, N2 adsorption-desorption isotherms and pore size distributions, additional CO2 adsorption isotherms and density functional theory model surfaces. This material is available free of charge via the Internet at http://pubs.acs.org.

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N2 - Solid metal oxides for carbon capture exhibit reduced adsorption capacity following high-temperature exposure, due to surface area reduction by sintering. Furthermore, only low-coordinate corner/edge sites on the thermodynamically stable (100) facet display favorable binding toward CO2, providing inherently low capacity. The (111) facet, however, exhibits a high concentration of low-coordinate sites. In this work, MgO(111) nanosheets displayed high capacity for CO2, as well as a ∼65% increase in capacity despite a ∼30% reduction in surface area following sintering (0.77 mmol g–1 @ 227 m2 g–1 vs 1.28 mmol g–1 @ 154 m2 g–1). These results, unique to MgO(111), suggest intrinsic differences in the effects of sintering on basic site retention. Spectroscopic and computational investigations provided a new structure–activity insight: the importance of high-temperature activation to unleash the capacity of the polar (111) facet of MgO. In summary, we present the first example of a faceted sorbent for carbon capture and challenge the assumption that sintering is necessarily a negative process; here we leverage high-temperature conditions for facet-dependent surface activation.

AB - Solid metal oxides for carbon capture exhibit reduced adsorption capacity following high-temperature exposure, due to surface area reduction by sintering. Furthermore, only low-coordinate corner/edge sites on the thermodynamically stable (100) facet display favorable binding toward CO2, providing inherently low capacity. The (111) facet, however, exhibits a high concentration of low-coordinate sites. In this work, MgO(111) nanosheets displayed high capacity for CO2, as well as a ∼65% increase in capacity despite a ∼30% reduction in surface area following sintering (0.77 mmol g–1 @ 227 m2 g–1 vs 1.28 mmol g–1 @ 154 m2 g–1). These results, unique to MgO(111), suggest intrinsic differences in the effects of sintering on basic site retention. Spectroscopic and computational investigations provided a new structure–activity insight: the importance of high-temperature activation to unleash the capacity of the polar (111) facet of MgO. In summary, we present the first example of a faceted sorbent for carbon capture and challenge the assumption that sintering is necessarily a negative process; here we leverage high-temperature conditions for facet-dependent surface activation.

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