2020
DOI: 10.1021/acs.jpca.0c08198
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Solid-State 17O NMR Studies of Sulfonate Jump Dynamics in Crystalline Sulfonic Acids: Insights into the Hydrogen Bonding Effect

Abstract: We report variable-temperature (VT) 17O solid-state nuclear magnetic resonance (NMR) spectra for three crystalline sulfonic acids: l-cysteic acid monohydrate (CA), 3-pyridinesulfonic acid (PSA), and p-toluenesulfonic acid monohydrate (TSA). We were able to analyze the experimental VT 17O NMR spectra to obtain the activation barriers for SO3 – jumps in these systems. Using the density functional-based tight-binding (DFTB) method, we performed potential energy surface scans for SO3 – jumps in the crystal lattice… Show more

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Cited by 12 publications
(6 citation statements)
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“…However, in the past few years, several approaches have been reported to address these obstacles. First, new methods to 17 O label peptides and carbohydrates using synthetic and acid-catalyzed exchange methods have been reported. Notably, 17 O labeled amino acids have been selectively incorporated into recombinant proteins making 17 O NMR feasible for biomacromolecules. , Recently, mechanochemistry has also been shown to be a robust and economic method for 17 O enrichment of a variety of compounds. Second, higher field NMR magnets and instrumentation have also contributed greatly to facilitating 17 O NMR spectroscopy. Magnetic fields up to 35.2 T have provided dramatic enhancements in spectral resolution and sensitivity through reduction of the second-order quadrupolar broadening, as illustrated in spectra of peptides and metal–organic frameworks (MOFs). ,,,, Third, cryogenic magic-angle spinning (MAS) probes and dynamic nuclear polarization have recently been used to yield a multifold increase in much needed spectral sensitivity. ,, Finally, solid-state NMR methods such as multiple-quantum magic-angle spinning (MQMAS) and satellite-transition magic-angle spinning (STMAS) which provide high-resolution isotropic spectra of half-integer quadrupolar nuclei are becoming increasingly popular for 17 O experiments.…”
mentioning
confidence: 99%
“…However, in the past few years, several approaches have been reported to address these obstacles. First, new methods to 17 O label peptides and carbohydrates using synthetic and acid-catalyzed exchange methods have been reported. Notably, 17 O labeled amino acids have been selectively incorporated into recombinant proteins making 17 O NMR feasible for biomacromolecules. , Recently, mechanochemistry has also been shown to be a robust and economic method for 17 O enrichment of a variety of compounds. Second, higher field NMR magnets and instrumentation have also contributed greatly to facilitating 17 O NMR spectroscopy. Magnetic fields up to 35.2 T have provided dramatic enhancements in spectral resolution and sensitivity through reduction of the second-order quadrupolar broadening, as illustrated in spectra of peptides and metal–organic frameworks (MOFs). ,,,, Third, cryogenic magic-angle spinning (MAS) probes and dynamic nuclear polarization have recently been used to yield a multifold increase in much needed spectral sensitivity. ,, Finally, solid-state NMR methods such as multiple-quantum magic-angle spinning (MQMAS) and satellite-transition magic-angle spinning (STMAS) which provide high-resolution isotropic spectra of half-integer quadrupolar nuclei are becoming increasingly popular for 17 O experiments.…”
mentioning
confidence: 99%
“…, in the absence of atomic motion). 69–77 Taking into account the ω Q (2) RL values for Na1 and Na2 in NaGaPO 4 F and the temperature range of motional changes in the 23 Na NMR spectrum, we can evaluate τ d −1 ∼ 10 3 –10 4 s −1 at T ≈ 300–350 K.…”
Section: Resultsmentioning
confidence: 99%
“…In particular, the motional changes in the NMR spectrum can be expected at temperatures at which the ion jump frequency, τ d −1 , becomes comparable with the characteristic frequency of the interaction determining the NMR line shape in a "rigid lattice" (i.e., in the absence of atomic motion). [69][70][71][72][73][74][75][76][77] Taking into account the ω Q…”
Section: Dalton Transactions Papermentioning
confidence: 99%
“…No change in the chemical shift would in turn suggest that no interaction takes place. Since the sulfonate charge-tagged complex [F e TMS (CO) 3 -SO 3 ]­Na contains no nuclei that can give conclusive information about the tag binding to iron ( 1 H, 13 C, 29 Si, 14 N/ 15 N) or nuclei that are cumbersome to work with and/or very expensive to enrich ( 57 Fe, 17 O, 33 S), we decided to prepare an “NMR-tagged” derivative. The next closest analogues to sulfonates are selenonates, which would offer 77 Se NMR (S = 1/2, 7.6% natural abundance) as a diagnostic tool.…”
Section: Discussionmentioning
confidence: 99%