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Title: Monitoring solvent dynamics and ion associations in the formation of cubic octamer polyanion in tetramethylammonium silicate solutions

Abstract

NMR methods were utilized to monitor the in situ structural and dynamic changes of various species in highly alkaline tetramethylammonium (TMA) silicate solutions. Quantitative 29Si NMR, 1H, 2H, and 17O relaxation NMR, and 1H and 29Si diffusion NMR of silicates, TMA, H2O and D2O demonstrate that the growth of the cubic octamer Q38 is accompanied by reduced water mobility and increasing TMA coordination number per Q38, which reaches an equilibrium value of 4.5 at 15 °C. Temperature-dependent measurements further reveal that the increased control over speciation by TMA at lower temperatures results from the more stable ion associations via slower solvent motions.


Citation Formats

Chen, Ying, Washton, Nancy M., Young, Robert P., Karkamkar, Abhijeet J., De Yoreo, James J., and Mueller, Karl T. Monitoring solvent dynamics and ion associations in the formation of cubic octamer polyanion in tetramethylammonium silicate solutions. United States: N. p., 2019. Web. doi:10.1039/C8CP07521B.
Chen, Ying, Washton, Nancy M., Young, Robert P., Karkamkar, Abhijeet J., De Yoreo, James J., & Mueller, Karl T. Monitoring solvent dynamics and ion associations in the formation of cubic octamer polyanion in tetramethylammonium silicate solutions. United States. doi:10.1039/C8CP07521B.
Chen, Ying, Washton, Nancy M., Young, Robert P., Karkamkar, Abhijeet J., De Yoreo, James J., and Mueller, Karl T. Thu . "Monitoring solvent dynamics and ion associations in the formation of cubic octamer polyanion in tetramethylammonium silicate solutions". United States. doi:10.1039/C8CP07521B.
@article{osti_1515852,
title = {Monitoring solvent dynamics and ion associations in the formation of cubic octamer polyanion in tetramethylammonium silicate solutions},
author = {Chen, Ying and Washton, Nancy M. and Young, Robert P. and Karkamkar, Abhijeet J. and De Yoreo, James J. and Mueller, Karl T.},
abstractNote = {NMR methods were utilized to monitor the in situ structural and dynamic changes of various species in highly alkaline tetramethylammonium (TMA) silicate solutions. Quantitative 29Si NMR, 1H, 2H, and 17O relaxation NMR, and 1H and 29Si diffusion NMR of silicates, TMA, H2O and D2O demonstrate that the growth of the cubic octamer Q38 is accompanied by reduced water mobility and increasing TMA coordination number per Q38, which reaches an equilibrium value of 4.5 at 15 °C. Temperature-dependent measurements further reveal that the increased control over speciation by TMA at lower temperatures results from the more stable ion associations via slower solvent motions.},
doi = {10.1039/C8CP07521B},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 9,
volume = 21,
place = {United States},
year = {2019},
month = {3}
}

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