Natural abundance 17O DNP two-dimensional and surface-enhanced NMR spectroscopy

Perras, Frédéric A.; Kobayashi, Takeshi; Pruski, Marek

doi:10.1021/jacs.5b03905

Natural abundance ¹⁷O DNP two-dimensional and surface-enhanced NMR spectroscopy

Journal Article · Mon Jun 22 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b03905· OSTI ID:1227378

Perras, Frédéric A. ^[1]; Kobayashi, Takeshi ^[1]; Pruski, Marek ^[2]

Ames Lab., Ames, IA (United States)
Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)

Due to its extremely low natural abundance and quadrupolar nature, the ¹⁷O nuclide is very rarely used for spectroscopic investigation of solids by NMR without isotope enrichment. Additionally, the applicability of dynamic nuclear polarization (DNP), which leads to sensitivity enhancements of 2 orders of magnitude, to ¹⁷O is wrought with challenges due to the lack of spin diffusion and low polarization transfer efficiency from ¹H. Here, we demonstrate new DNP-based measurements that extend ¹⁷O solid-state NMR beyond its current capabilities. The use of the PRESTO technique instead of conventional ¹H–¹⁷O cross-polarization greatly improves the sensitivity and enables the facile measurement of undistorted line shapes and two-dimensional ¹H–¹⁷O HETCOR NMR spectra as well as accurate internuclear distance measurements at natural abundance. This was applied for distinguishing hydrogen-bonded and lone ¹⁷O sites on the surface of silica gel; the one-dimensional spectrum of which could not be used to extract such detail. As a result, this greatly enhanced sensitivity has enabled, for the first time, the detection of surface hydroxyl sites on mesoporous silica at natural abundance, thereby extending the concept of DNP surface-enhanced NMR spectroscopy to the ¹⁷O nuclide.

View Accepted Manuscript (DOE)

Research Organization:: Ames Laboratory (AMES), Ames, IA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-07CH11358

OSTI ID:: 1227378

Report Number(s):: IS-J--8740

Journal Information:: Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 26 Vol. 137; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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