Structural information from quadrupolar nuclei in solid state NMR

Ashbrook, Sharon E.; Duer, Melinda J.

doi:10.1002/cmr.a.20053

Cited by 146 publications

(268 citation statements)

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“…When the calcium is not in a highly symmetric environment, i.e. as in cubic calcium oxide, the observed signal of the central transition is commonly broadened by the second order quadrupolar interaction, 45,46 drastically reducing the intensity of the signals. An additional complication commonly encountered in solid state NMR of low-g nuclei is rather long relaxation times.…”

Section: Introductionmentioning

confidence: 99%

Natural abundance high field 43Ca solid state NMR in cement science

Moudrakovski

Alizadeh

Beaudoin

2010

Phys. Chem. Chem. Phys.

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/npsi/ctrl?lang=en http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/ctrl?lang=fr Access and use of this website and the material on it are subject to the Terms and Conditions set forth at http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/jsp/nparc_cp.jsp?lang=en NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. For the publisher's version, please access the DOI link below./ Pour consulter la version de l'éditeur, utilisez le lien DOI ci-dessous.http://dx.doi.org/10.1039/c000353kPhysical Chemistry Chemical Physics, 12, pp. 6961-6969, 2010-06-01 Natural abundance high field 43Ca NMR solid state NMR in cement science Moudrakovski, I.; Alizadeh, R.; Beaudoin, J. J. The material in this document is covered by the provisions of the Copyright Act, by Canadian laws, policies, regulations and international agreements. Such provisions serve to identify the information source and, in specific instances, to prohibit reproduction of materials without written permission. For more information visit http://laws.justice.gc.ca/en/showtdm/cs/C-42Les renseignements dans ce document sont protégés par la Loi sur le droit d'auteur, par les lois, les politiques et les règlements du Canada et des accords internationaux. Ces dispositions permettent d'identifier la source de l'information et, dans certains cas, d'interdire la copie de documents sans permission écrite. Pour obtenir de plus amples renseignements : http://lois.justice.gc.ca/fr/showtdm/cs/C-42 Natural abundance high field 43 Ca solid state NMR in cement sciencew This work is a systematic attempt to determine the possibilities and the limitations of the 43 Ca high field solid state NMR in the study of cement-based materials. The low natural abundance (0.135%) and small gyromagnetic ratio of 43 Ca present a serious challenge even in a high magnetic field. The NMR spectra of a number of cement compounds of known structure and composition are examined. The spectra of several phases important in cement science, e.g., anhydrous beta di-calcium silicate (b-C 2 S) and tri-calcium (C 3 S) silicate were obtained for the first time and the relation of spectroscopic and structural parameters is discussed. The method was also applied to the hydrated C 3 S and synthetic calcium silicate hydrates (C-S-H) of different composition in order to understand the state of calcium and transformations in the structure during hydrolysis. The spectra of hydrated C 3 S reveals a calcium environment similar to that of the C-S-H samples and 11 Å Tobermorite. These observations support the validity of using layered crystalline C-S-H systems as structural models for the C-S-H that forms in the hydration of Portland cement.

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Section: Introductionmentioning

confidence: 99%

Natural abundance high field 43Ca solid state NMR in cement science

Moudrakovski

Alizadeh

Beaudoin

2010

Phys. Chem. Chem. Phys.

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“…A variety of techniques have been developed for the rapid and efficient acquisition of quadrupolar-dominated powder patterns. [1][2][3][4] Recently, much work has been dedicated to the SSNMR spectroscopy of unreceptive quadrupolar nuclei (e.g., 79 Br, 127 I, 209 Bi, 115 In, 73 Ge, 14 N, 33 S, 87 Sr, 25 Mg, 43 Ca, etc. ), [5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] which are defined as nuclei which may have low gyromagnetic ratios, low natural abundances, broad anisotropic patterns, long relaxation times, or combinations of these characteristics.…”

Section: Introductionmentioning

confidence: 99%

Solid-State ¹³⁷Ba NMR Spectroscopy: An Experimental and Theoretical Investigation of ¹³⁷Ba Electric Field Gradient Tensors and Their Relation to Structure and Symmetry

Hamaed

Udachin

et al. 2010

J. Phys. Chem. B

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Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions? Contact the NRC Publications Archive team atPublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/eng/view/object/?id=4daed0b0-5d6e-4f41-9df3-c6915e17e8b5 http://nparc.cisti-icist.nrc-cnrc.gc.ca/fra/voir/objet/?id=4daed0b0-5d6e-4f41-9df3-c6915e17e8b5 Ba SSNMR spectra of several barium-containing systems (barium nitrate, barium carbonate, barium chlorate monohydrate, barium chloride dihydrate, anhydrous barium chloride, and barium hydrogen phosphate) were acquired at two different magnetic field strengths (9.4 and 21.1 T) using frequency-stepped techniques. The recently reported WURST-QCPMG pulse sequence (O'Dell et al. Chem. Phys. Lett. 2008, 464,9 7 -102) is shown to be very useful for rapidly acquiring high signal-to-noise 137 Ba SSNMR spectra. The breadths of the second-order quadrupolar-dominated spectra and experimental times are notably reduced for experiments conducted at 21.1 T. Ba electric field gradient (EFG) parameters extracted from these spectra are correlated to the local environments at the barium sites, via consideration of molecular symmetry and structure, and first principles calculations of 137 Ba EFG tensors performed using CASTEP software. The rapidity with which 137 Ba SSNMR spectra can be acquired using the WURST pulse sequence and/or at ultrahigh magnetic fields and the sensitivity of the 137 Ba EFG tensor parameters to the changes in the barium environment suggest that 137 Ba SSNMR has great potential for structural characterization of a variety of barium-containing materials.

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“…Ashbrook and Duer have recently described in detail how structural information may be extracted from solid-state NMR experiments performed on quadrupolar nuclei. 21 Motivated by their review, we present here a new cross-validation approach to determine the quality of quantum chemically optimized hydrogen-bonded proton positions, which uses the experimental chlorine quadrupolar coupling data.…”

Section: Introductionmentioning

confidence: 99%

“…Ashbrook and Duer have recently described in detail how structural information may be extracted from solid-state NMR experiments performed on quadrupolar nuclei. 21 Motivated by their review, we present here a new cross-* Author to whom correspondence should be addressed. E-mail dbryce@uottawa.ca.…”

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confidence: 99%

Chlorine-35/37 NMR Spectroscopy of Solid Amino Acid Hydrochlorides: Refinement of Hydrogen-Bonded Proton Positions Using Experiment and Theory

2006

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Trends in the chlorine chemical shift (CS) tensors of amino acid hydrochlorides are investigated in the context of new data obtained at 21.1 T and extensive quantum chemical calculations. The analysis of chlorine-35/37 NMR spectra of solid L-tryptophan hydrochloride obtained at two magnetic field strengths yields the chlorine electric field gradient (EFG) and CS tensors, and their relative orientations. The chlorine CS tensor is also determined for the first time for DL-arginine hydrochloride monohydrate. The drastic influence of 1 H decoupling at 21.1 T on the spectral features of salts with particularly small 35 Cl quadrupolar coupling constants (C Q ) is demonstrated. The chlorine CS tensor spans (Ω) of hydrochloride salts of hydrophobic amino acids are found to be larger than those for salts of hydrophilic amino acids. A new combined experimental-theoretical procedure is described in which quantum chemical geometry optimizations of hydrogen-bonded proton positions around the chloride ions in a series of amino acid hydrochlorides are cross-validated against the experimental chlorine EFG and CS tensor data. The conclusion is reached that the relatively computationally inexpensive B3LYP/ 3-21G* method provides proton positions which are suitable for subsequent higher-level calculations of the chlorine EFG tensors. The computed value of Ω is less sensitive to the proton positions. Following this cross-validation procedure, |C Q ( 35 Cl)| is generally predicted within 15% of the experimental value for a range of HCl salts. The results suggest the applicability of chlorine NMR interaction tensors in the refinement of proton positions in structurally similar compounds, e.g., chloride ion channels, for which neutron diffraction data are unavailable. IntroductionThe availability of high-field solid-state nuclear magnetic resonance (NMR) spectrometers, e.g., those with 1 H resonance frequencies of 800 MHz, 900 MHz, and above, has created new opportunities for the study of quadrupolar nuclei (I > 1/ 2) with low resonance frequencies or large quadrupole moments, and for nuclei with both of these properties. For example, Stebbins et al. have described applications of 18.8 and 21.1 T solid-state 27 Al, 17 O, 39 K, and 35 Cl NMR spectroscopy to study oxide materials. 1-3 Gan et al. used magnetic fields as high as 40 T to achieve chemical shift resolution between four different aluminum environments in aluminoborate. 4 Ellis and colleagues have applied high-field 67 Zn NMR at low temperature to study zinc binding environments of biological relevance. 5,6,7,8 Magicangle-spinning (MAS) NMR in a magnetic field of 19.6 T has been applied by Wu and co-workers to detect potassium cations in guanine-quadruplex structures 9 as well as to explore cation-π interactions in alkali metal tetraphenylborates. 10 Cross and coworkers have demonstrated the utility of 17 O solid-state NMR at 21.1 T for characterizing the ion channel gramicidin. 11,12 The major reason that higher fields are so beneficial for the study of quadrupolar nuclei in ...

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Structural information from quadrupolar nuclei in solid state NMR

Cited by 146 publications

References 182 publications

Natural abundance high field 43Ca solid state NMR in cement science

Natural abundance high field 43Ca solid state NMR in cement science

Solid-State ¹³⁷Ba NMR Spectroscopy: An Experimental and Theoretical Investigation of ¹³⁷Ba Electric Field Gradient Tensors and Their Relation to Structure and Symmetry

Chlorine-35/37 NMR Spectroscopy of Solid Amino Acid Hydrochlorides: Refinement of Hydrogen-Bonded Proton Positions Using Experiment and Theory

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Structural information from quadrupolar nuclei in solid state NMR

Cited by 146 publications

References 182 publications

Natural abundance high field 43Ca solid state NMR in cement science

Natural abundance high field 43Ca solid state NMR in cement science

Solid-State 137Ba NMR Spectroscopy: An Experimental and Theoretical Investigation of 137Ba Electric Field Gradient Tensors and Their Relation to Structure and Symmetry

Chlorine-35/37 NMR Spectroscopy of Solid Amino Acid Hydrochlorides: Refinement of Hydrogen-Bonded Proton Positions Using Experiment and Theory

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Solid-State ¹³⁷Ba NMR Spectroscopy: An Experimental and Theoretical Investigation of ¹³⁷Ba Electric Field Gradient Tensors and Their Relation to Structure and Symmetry