title: In situ studies of materials for high temperature CO2capture and storage.
abstract: Carbon capture and storage (CCS) offers a possible solution to curb the CO2emissions from stationary sources in the coming decades, considering the delays in shifting energy generation to carbon neutral sources such as wind, solar and biomass. The most mature technology for post-combustion capture uses a liquid sorbent, amine scrubbing. However, with the existing technology, a large amount of heat is required for the regeneration of the liquid sorbent, which introduces a substantial energy penalty. The use of alternative sorbents for CO2capture, such as the CaO-CaCO3system, has been investigated extensively in recent years. However there are significant problems associated with the use of CaO based sorbents, the most challenging one being the deactivation of the sorbent material. When sorbents such as natural limestone are used, the capture capacity of the solid sorbent can fall by as much as 90 mol% after the first 20 carbonation-regeneration cycles. In this study a variety of techniques were employed to understand better the cause of this deterioration from both a structural and morphological standpoint. X-ray and neutron PDF studies were employed to understand better the local surface and interfacial structures formed upon reaction, finding that after carbonation the surface roughness is decreased for CaO. In situ synchrotron X-ray diffraction studies showed that carbonation with added steam leads to a faster and more complete conversion of CaO than under conditions without steam, as evidenced by the phases seen at different depths within the sample. Finally, in situ X-ray tomography experiments were employed to track the morphological changes in the sorbents during carbonation, observing directly the reduction in porosity and increase in tortuosity of the pore network over multiple calcination reactions.
authors.affiliation: Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK. cpg27@cam.ac.uk.
authors.forename: Matthew T
authors.initials: MT
authors.lastname: Dunstan
authors.affiliation: School of Physics and Astronomy, Queen Mary University of London, London E1 4NS, UK.
authors.forename: Serena A
authors.initials: SA
authors.lastname: Maugeri
authors.affiliation: Cambridge Centre for Advanced Research and Education in Singapore, Nanyang Technological University, 1 Create Way, Singapore 138602.
authors.forename: Wen
authors.initials: W
authors.lastname: Liu
authors.affiliation: ISIS Facility, Rutherford Appleton Laboratory, Harwell Campus, Didcot OX11 0QX, UK and Diamond Light Source, Chilton, Oxfordshire OX11 0DE, UK and Spallation Neutron Source, Oak Ridge National Laboratory, Oak Ridge, USA.
authors.forename: Matthew G
authors.initials: MG
authors.lastname: Tucker
authors.affiliation: Department of Chemical Engineering, University College London, London WC1E 7JE, UK.
authors.forename: Oluwadamilola O
authors.initials: OO
authors.lastname: Taiwo
authors.affiliation: Department of Chemical Engineering and Biotechnology, University of Cambridge, Pembroke Street, Cambridge, CB2 3RA, UK.
authors.forename: Belen
authors.initials: B
authors.lastname: Gonzalez
authors.affiliation: Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK. cpg27@cam.ac.uk.
authors.forename: Phoebe K
authors.initials: PK
authors.lastname: Allan
authors.affiliation: Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK. cpg27@cam.ac.uk.
authors.forename: Michael W
authors.identifier: 0000-0003-2172-2507
authors.initials: MW
authors.lastname: Gaultois
authors.affiliation: Department of Chemical Engineering, University College London, London WC1E 7JE, UK.
authors.forename: Paul R
authors.initials: PR
authors.lastname: Shearing
authors.affiliation: ISIS Facility, Rutherford Appleton Laboratory, Harwell Campus, Didcot OX11 0QX, UK.
authors.forename: David A
authors.initials: DA
authors.lastname: Keen
authors.affiliation: School of Physics and Astronomy, Queen Mary University of London, London E1 4NS, UK.
authors.forename: Anthony E
authors.initials: AE
authors.lastname: Phillips
authors.affiliation: School of Physics and Astronomy, Queen Mary University of London, London E1 4NS, UK.
authors.forename: Martin T
authors.initials: MT
authors.lastname: Dove
authors.affiliation: Department of Engineering, University of Cambridge, Trumpington Street, Cambridge CB2 1PZ, UK.
authors.forename: Stuart A
authors.initials: SA
authors.lastname: Scott
authors.affiliation: Department of Chemical Engineering and Biotechnology, University of Cambridge, Pembroke Street, Cambridge, CB2 3RA, UK.
authors.forename: John S
authors.initials: JS
authors.lastname: Dennis
authors.affiliation: Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK. cpg27@cam.ac.uk.
authors.forename: Clare P
authors.initials: CP
authors.lastname: Grey