ORCID

http://orcid.org/0000-0002-9304-4330

Date of Award

Summer 8-15-2019

Author's School

Graduate School of Arts and Sciences

Author's Department

Chemistry

Degree Name

Doctor of Philosophy (PhD)

Degree Type

Dissertation

Abstract

The work described in this dissertation has been accomplished by using solid-state nuclear magnetic resonance (SSNMR) spectroscopy to investigate CO2 mineralization and to refine the positions of protons in the crystalline system. The reaction of forsterite (Mg2SiO4) and 13CO2 is presented here, which is measured using in-situ 13C NMR spectroscopy without removing the sample from the reactor. 29Si SSNMR is used to investigate the reaction of forsterite with 13CO2 in the presence of water or NaCl brine as a function of depth in the sample. Additionally, we also show that NMR crystallography can significantly improve structure refinement of hydrogens’ positions in hydrated materials. 13C{1H} rotational-echo double-resonance (REDOR) and 13C chemical shift anisotropy (CSA) tensor values from SSNMR are exploited as the standard in NMR crystallography. The optimized atomic coordinates are validated by comparing DFT prediction to experimental data through 13C{1H} REDOR and 13C CSA tensors. The research presented herein demonstrates that solid-state NMR is a useful tool for studying the CO2 mineralization mechanism and the understanding of the crystalline structure of CO2 mineralization products.

Language

English (en)

Chair and Committee

Sophia E. Hayes

Committee Members

Alexander Barnes, Julio M. D'Arcy, Joseph A. Fournier, Jill D. Pasteris,

Comments

Permanent URL: https://doi.org/10.7936/0kf8-cr83

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