CO2-mineralization and carbonation reactor rig: Design and validation for in situ neutron scattering experiments-Engineering and lessons learned

Ali Mortazavi; Fu Song; Michael Dudman; Michael Evans; Robert Copcutt; Giovanni Romanelli; Franz Demmel; David H Farrar; Stewart F Parker; Kun V Tian; Devis Di Tommaso; Gregory A Chass

doi:10.1063/5.0136204

CO2-mineralization and carbonation reactor rig: Design and validation for in situ neutron scattering experiments-Engineering and lessons learned

Rev Sci Instrum. 2023 Sep 1;94(9):093905. doi: 10.1063/5.0136204.

Authors

Ali Mortazavi¹, Fu Song², Michael Dudman¹, Michael Evans³, Robert Copcutt³, Giovanni Romanelli⁴, Franz Demmel¹, David H Farrar⁵, Stewart F Parker¹, Kun V Tian^{5

6

7}, Devis Di Tommaso², Gregory A Chass^{2

5

6}

Affiliations

¹ ISIS Neutron and Muon Facility, STFC Rutherford Appleton Laboratory, Harwell OX14 0QX, United Kingdom.
² Department of Chemistry, School of Physical and Chemical Sciences, Queen Mary University of London, London E1 4NS, United Kingdom.
³ Cambridge Carbon Capture, Cambridge, United Kingdom.
⁴ Department of Physics, University of Rome Tor Vergata, via della Ricerca Scientifica 1, 00133 Roma, Italy.
⁵ Department of Chemistry, McMaster University, Hamilton, Ontario L8S 4L8, Canada.
⁶ Faculty of Land and Food Systems, The University of British Columbia, Vancouver, British Columbia V6T1Z4, Canada.
⁷ Department of Chemistry and Pharmaceutical Sciences, Sapienza University of Rome, Piazzale Aldo Moro, 5, 00185 Roma, Italy.

PMID: 37724925
DOI: 10.1063/5.0136204

Abstract

CO2 mineralization via aqueous Mg/Ca/Na-carbonate (MgCO3/CaCO3/Na2CO3) formation represents a huge opportunity for the utilization of captured CO2. However, large-scale mineralization is hindered by slow kinetics due to the highly hydrated character of the cations in aqueous solutions (Mg2+ in particular). Reaction conditions can be optimized to accelerate carbonation kinetics, for example, by the inclusion of additives that promote competitive dehydration of Mg2+ and subsequent agglomeration, nucleation, and crystallization. For tracking mineralization and these reaction steps, neutron scattering presents unprecedented advantages over traditional techniques for time-resolved in situ measurements. However, a setup providing continuous solution circulation to ensure reactant system homogeneity for industrially relevant CO2-mineralization is currently not available for use on neutron beamlines. We, therefore, undertook the design, construction, testing and implementation of such a self-contained reactor rig for use on selected neutron beamlines at the ISIS Neutron and Muon Source (Harwell, UK). The design ensured robust attachment via suspension from the covering Tomkinson flange to stabilize the reactor assembly and all fittings (~25 kg), as well as facilitating precise alignment of the entire reactor and sample (test) cell with respect to beam dimension and direction. The assembly successfully accomplished the principal tasks of providing a continuous flow of the reaction mixture (~500 mL) for homogeneity, quantitative control of CO2 flux into the mixture, and temperature and pressure regulation throughout the reaction and measurements. The design is discussed, with emphasis placed on the reactor, including its geometry, components, and all technical specifications. Descriptions of the off-beamline bench tests, safety, and functionality, as well as the installation on beamlines and trial experimental procedure, are provided, together with representative raw neutron scattering results.