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Trapping amorphous intermediates of carbonates – a combined total scattering and NMR study

DOI: 10.1021/jacs.8b06703 DOI Help

Authors: Sebastian Leukel (Johannes Gutenberg-Universität Mainz; Graduate School Materials Science in Mainz) , Martin Panthöfer (Johannes Gutenberg-Universität Mainz) , Mihail Mondeshki (Johannes Gutenberg-Universität Mainz) , Gregor Kieslich (University of Cambridge) , Yue Wu (National University of Singapore) , Nina Krautwurst (Johannes Gutenberg Universitat Mainz) , Wolfgang Tremel (Johannes Gutenberg-Universität Mainz)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Journal Of The American Chemical Society

State: Published (Approved)
Published: October 2018
Diamond Proposal Number(s): 13843

Abstract: Crystallization via metastable phases plays an important role in chemical manufacturing, bio-mineralization, and protein crystallization, but the kinetic pathways leading from metastable phases to the stable crystalline modifications are not well understood. In particular, the fast crys-tallization of amorphous intermediates makes a detailed characterization challenging. To circum-vent this problem, we devised a system that allows trapping and stabilizing the amorphous in-termediates of representative carbonates (calcium, strontium, barium, manganese, and cadmium). The long-term stabilization of these transient species enabled a detailed investigation of their composition, structure, and morphology. Total scattering experiments with high-energy syn-chrotron radiation revealed a short-range order of several Ångström in all amorphous intermedi-ates. From the synchrotron data, a structural model of amorphous calcium carbonate was de-rived that indicates a lower coordination number of calcium compared to the crystalline poly-morphs. Our study shows that a multi-step crystallization pathway via amorphous intermediates is open to many carbonates. We could isolate and characterize these transient species, thereby providing new insights into their crystallization mechanism.

Journal Keywords: carbonate; amorphous; nanoparticles; crystallization

Subject Areas: Chemistry


Instruments: I15-Extreme Conditions