NMR Nanoparticle Diffusometry in Hydrogels: Enhancing Sensitivity and Selectivity

D.W. de Kort, J.P.M. van Duynhoven, F.J.M. Hoeben, H.M. Janssen, H. van As

Research output: Contribution to journalArticleAcademicpeer-review

11 Citations (Scopus)

Abstract

From the diffusional behavior of nanoparticles in heterogeneous hydrogels, quantitative information about submicron structural features of the polymer matrix can be derived. Pulsed-gradient spin-echo NMR is often the method of choice because it measures diffusion of the whole ensemble of nanoparticles. However, in 1H diffusion-ordered spectroscopy (DOSY), low-intensity nanoparticle signals have to be separated from a highly protonated background. To circumvent this, we prepared 19F labeled, PEGylated, water-soluble dendritic nanoparticles with a 19F loading of ~7 wt % to enable background free 19F DOSY experiments. 19F nanoparticle diffusometry was benchmarked against 1H diffusion-T2 correlation spectroscopy (DRCOSY), which has a stronger signal separation potential than the commonly used 1H DOSY experiment. We used bootstrap data resampling to estimate confidence intervals and stabilize 2D-Laplace inversion of DRCOSY data with high noise levels and artifacts, allowing quantitative diffusometry even at low magnetic field strengths (30 MHz). The employed methods offer significant advantages in terms of sensitivity and selectivity.
Original languageEnglish
Pages (from-to)9229-9235
JournalAnalytical Chemistry
Volume86
DOIs
Publication statusPublished - 2014

Fingerprint

Hydrogels
Nuclear magnetic resonance
Nanoparticles
Spectroscopy
Polymer matrix
Experiments
Magnetic fields
Water

Keywords

  • fluorescence recovery
  • laplace inversion
  • polymer-solutions
  • field gradient
  • diffusion
  • resolution
  • mobility
  • gels
  • spectroscopy
  • kinetics

Cite this

@article{504e11b47ae645e0a37ef25392993eb7,
title = "NMR Nanoparticle Diffusometry in Hydrogels: Enhancing Sensitivity and Selectivity",
abstract = "From the diffusional behavior of nanoparticles in heterogeneous hydrogels, quantitative information about submicron structural features of the polymer matrix can be derived. Pulsed-gradient spin-echo NMR is often the method of choice because it measures diffusion of the whole ensemble of nanoparticles. However, in 1H diffusion-ordered spectroscopy (DOSY), low-intensity nanoparticle signals have to be separated from a highly protonated background. To circumvent this, we prepared 19F labeled, PEGylated, water-soluble dendritic nanoparticles with a 19F loading of ~7 wt {\%} to enable background free 19F DOSY experiments. 19F nanoparticle diffusometry was benchmarked against 1H diffusion-T2 correlation spectroscopy (DRCOSY), which has a stronger signal separation potential than the commonly used 1H DOSY experiment. We used bootstrap data resampling to estimate confidence intervals and stabilize 2D-Laplace inversion of DRCOSY data with high noise levels and artifacts, allowing quantitative diffusometry even at low magnetic field strengths (30 MHz). The employed methods offer significant advantages in terms of sensitivity and selectivity.",
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author = "{de Kort}, D.W. and {van Duynhoven}, J.P.M. and F.J.M. Hoeben and H.M. Janssen and {van As}, H.",
year = "2014",
doi = "10.1021/ac502211q",
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journal = "Analytical Chemistry",
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NMR Nanoparticle Diffusometry in Hydrogels: Enhancing Sensitivity and Selectivity. / de Kort, D.W.; van Duynhoven, J.P.M.; Hoeben, F.J.M.; Janssen, H.M.; van As, H.

In: Analytical Chemistry, Vol. 86, 2014, p. 9229-9235.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - NMR Nanoparticle Diffusometry in Hydrogels: Enhancing Sensitivity and Selectivity

AU - de Kort, D.W.

AU - van Duynhoven, J.P.M.

AU - Hoeben, F.J.M.

AU - Janssen, H.M.

AU - van As, H.

PY - 2014

Y1 - 2014

N2 - From the diffusional behavior of nanoparticles in heterogeneous hydrogels, quantitative information about submicron structural features of the polymer matrix can be derived. Pulsed-gradient spin-echo NMR is often the method of choice because it measures diffusion of the whole ensemble of nanoparticles. However, in 1H diffusion-ordered spectroscopy (DOSY), low-intensity nanoparticle signals have to be separated from a highly protonated background. To circumvent this, we prepared 19F labeled, PEGylated, water-soluble dendritic nanoparticles with a 19F loading of ~7 wt % to enable background free 19F DOSY experiments. 19F nanoparticle diffusometry was benchmarked against 1H diffusion-T2 correlation spectroscopy (DRCOSY), which has a stronger signal separation potential than the commonly used 1H DOSY experiment. We used bootstrap data resampling to estimate confidence intervals and stabilize 2D-Laplace inversion of DRCOSY data with high noise levels and artifacts, allowing quantitative diffusometry even at low magnetic field strengths (30 MHz). The employed methods offer significant advantages in terms of sensitivity and selectivity.

AB - From the diffusional behavior of nanoparticles in heterogeneous hydrogels, quantitative information about submicron structural features of the polymer matrix can be derived. Pulsed-gradient spin-echo NMR is often the method of choice because it measures diffusion of the whole ensemble of nanoparticles. However, in 1H diffusion-ordered spectroscopy (DOSY), low-intensity nanoparticle signals have to be separated from a highly protonated background. To circumvent this, we prepared 19F labeled, PEGylated, water-soluble dendritic nanoparticles with a 19F loading of ~7 wt % to enable background free 19F DOSY experiments. 19F nanoparticle diffusometry was benchmarked against 1H diffusion-T2 correlation spectroscopy (DRCOSY), which has a stronger signal separation potential than the commonly used 1H DOSY experiment. We used bootstrap data resampling to estimate confidence intervals and stabilize 2D-Laplace inversion of DRCOSY data with high noise levels and artifacts, allowing quantitative diffusometry even at low magnetic field strengths (30 MHz). The employed methods offer significant advantages in terms of sensitivity and selectivity.

KW - fluorescence recovery

KW - laplace inversion

KW - polymer-solutions

KW - field gradient

KW - diffusion

KW - resolution

KW - mobility

KW - gels

KW - spectroscopy

KW - kinetics

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JF - Analytical Chemistry

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