Carbonates; Nucleation Theory; Calcium; Magnesium; Water; Aerosol; Crystallization; Synchrotron; XAS; EXAFS; carbon capture and Storage ; CCS; Global warming; Carbon dioxide; geological carbon cycle ; material synthesis
Xto Jacinta, Wetter Reto, Borca Camelia N., Frieh Christophe, van Bokhoven Jeroen A., Huthwelker Thomas (2019), Droplet-based in situ X-ray absorption spectroscopy cell for studying crystallization processes at the tender X-ray energy range, in RSC Advances
, 9(58), 34004-34010.
Xto Jacinta M., Borca Camelia N., van Bokhoven Jeroen A., Huthwelker Thomas (2019), Aerosol-based synthesis of pure and stable amorphous calcium carbonate, in Chemical Communications
, 55(72), 10725-10728.
Xto Jacinta M., Du Huachuan, Borca Camelia N., Amstad Esther, van Bokhoven Jeroen A., Huthwelker Thomas (2019), Tuning the Incorporation of Magnesium into Calcite during Its Crystallization from Additive-Free Aqueous Solution, in Crystal Growth & Design
, 19(8), 4385-4394.
Curti Enzo, Xto Jacinta, Borca Camelia N., Henzler Katja, Huthwelker Thomas, Prasianakis Nikolaos I. (2019), Modelling Ra-bearing baryte nucleation/precipitation kinetics at the pore scale: application to radioactive waste disposalModelling Ra-bearing baryte nucleation/precipitation kinetics at the pore scale: application to radioactive waste disposal, in European Journal of Mineralogy
, 31(2), 247-262.
Henzler Katja, Fetisov Evgenii O., Galib Mirza, Baer Marcel D., Legg Benjamin A., Borca Camelia, Xto Jacinta M., Pin Sonia, Fulton John L., Schenter Gregory K., Govind Niranjan, Siepmann J. Ilja, Mundy Christopher J., Huthwelker Thomas, De Yoreo James J. (2018), Supersaturated calcium carbonate solutions are classical, in Science Advances
, 4(1), eaao6283-eaao6283.
As main reservoir of the earth’s CO2, carbonates are key to the global carbon cycle, and the industrial synthesis of carbonates to bind anthropogenic CO2 is discussed as carbon storage technique. As main constituent of often nanostructured biominerals, carbonates can be considered as model materials for new functional materials. The precipitation of carbonates from aqueous solutions follows a multistep process via amorphous carbonate clusters (ACC) as intermediates, which have also been found as in biominerals. The stability of ACC is still an open question, and the presence of organics, silicate and magnesium has been shown to stabilize ACC. The mechanism how magnesium incorporates into ACC is unclear, but recent studies indicate that a dehydrated environment supports the synthesis of magnesium enriched ACC. ACC contain about 50 % of water molecules, and their dehydration is the key step towards crystallization of the ACC. Here we propose to synthesize ACC from airborne microdroplets, which contain calcium and magnesium in various composition. The microdroplets will be processed in a gas flow system under controlled conditions of temperature and gas phase (humidity and CO2 partial pressure), and then deposited into an in situ cell for spectroscopic studies of the ACC dehydration under controlled conditions (i.e. temperature, gas phase). Spectroscopic analysis will be made by IR spectroscopy, diffraction and synchrotron based x-ray absorption spectroscopy. Aim of the study is to relate the conditions of dehydration to the crystallization products and to study the structural changes in the ACC during dehydration. In a related project there will be studies on the structure of super saturated solutions of magnesium carbonates and also of salt solutions such as MgSO4, to understand the solution structure, and hence the process just before the nucleation in a solution occurs.