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Title: Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel

Engineering nanoparticle (NP) functions at the molecular level requires a detailed understanding of the dynamic processes occurring at the NP surface. Herein we show that a combination of dark-state exchange saturation transfer (DEST) and relaxation dispersion (RD) NMR experiments on gel-stabilized NP samples enables the accurate determination of the kinetics and thermodynamics of adsorption. We used the former approach to describe the interaction of cholic acid (CA) and phenol (PhOH) with ceria NPs with a diameter of approximately 200 nm. Whereas CA formed weak interactions with the NPs, PhOH was tightly bound to the NP surface. Interestingly, we found that the adsorption of PhOH proceeds via an intermediate, weakly bound state in which the small molecule has residual degrees of rotational diffusion. Here we believe the use of aqueous gels for stabilizing NP samples will increase the applicability of solution NMR methods to the characterization of nanomaterials.
Authors:
 [1] ;  [2] ;  [2] ;  [2] ;  [1]
  1. Iowa State Univ., Ames, IA (United States)
  2. Ames Lab. and Iowa State Univ., Ames, IA (United States)
Publication Date:
Report Number(s):
IS-J-9437
Journal ID: ISSN 1433-7851
Grant/Contract Number:
AC02-07CH11358
Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 33; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Research Org:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1379202
Alternate Identifier(s):
OSTI ID: 1378297

Egner, Timothy K., Naik, Pranjali, Nelson, Nicholas C., Slowing, Igor I., and Venditti, Vincenzo. Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel. United States: N. p., Web. doi:10.1002/anie.201704471.
Egner, Timothy K., Naik, Pranjali, Nelson, Nicholas C., Slowing, Igor I., & Venditti, Vincenzo. Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel. United States. doi:10.1002/anie.201704471.
Egner, Timothy K., Naik, Pranjali, Nelson, Nicholas C., Slowing, Igor I., and Venditti, Vincenzo. 2017. "Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel". United States. doi:10.1002/anie.201704471. https://www.osti.gov/servlets/purl/1379202.
@article{osti_1379202,
title = {Mechanistic Insight into Nanoparticle Surface Adsorption by Solution NMR Spectroscopy in an Aqueous Gel},
author = {Egner, Timothy K. and Naik, Pranjali and Nelson, Nicholas C. and Slowing, Igor I. and Venditti, Vincenzo},
abstractNote = {Engineering nanoparticle (NP) functions at the molecular level requires a detailed understanding of the dynamic processes occurring at the NP surface. Herein we show that a combination of dark-state exchange saturation transfer (DEST) and relaxation dispersion (RD) NMR experiments on gel-stabilized NP samples enables the accurate determination of the kinetics and thermodynamics of adsorption. We used the former approach to describe the interaction of cholic acid (CA) and phenol (PhOH) with ceria NPs with a diameter of approximately 200 nm. Whereas CA formed weak interactions with the NPs, PhOH was tightly bound to the NP surface. Interestingly, we found that the adsorption of PhOH proceeds via an intermediate, weakly bound state in which the small molecule has residual degrees of rotational diffusion. Here we believe the use of aqueous gels for stabilizing NP samples will increase the applicability of solution NMR methods to the characterization of nanomaterials.},
doi = {10.1002/anie.201704471},
journal = {Angewandte Chemie (International Edition)},
number = 33,
volume = 56,
place = {United States},
year = {2017},
month = {6}
}