Publication Date

1-2018

Department

Ames Laboratory; Materials Science and Engineering; Chemistry

Campus Units

Chemistry, Materials Science and Engineering, Ames Laboratory

Report Number

IS-J 9394

DOI

10.1016/j.cocis.2017.11.002

Journal Title

Current Opinion in Colloid & Interface Science

Volume Number

33

First Page

9

Last Page

18

Abstract

The efficacy of dynamic nuclear polarization (DNP) surface-enhanced NMR spectroscopy (SENS) is reviewed for alumina, silica, and ordered mesoporous carbon (OMC) materials, with vastly different surface areas, as a function of the biradical concentration. Importantly, our studies show that the use of a “one-size-fits-all” biradical concentration should be avoided when performing DNP SENS experiments and instead an optimal concentration should be selected as appropriate for the type of material studied as well as its surface area. In general, materials with greater surface areas require higher radical concentrations for best possible DNP performance. This result is explained with the use of a thermodynamic model wherein radical-surface interactions are expected to lead to an increase in the local concentration of the polarizing agent at the surface. We also show, using plane-wave density functional theory calculations, that weak radical-surface interactions are the cause of the poor performance of DNP SENS for carbonaceous materials.

Language

en

Department of Energy Subject Categories

36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 47 OTHER INSTRUMENTATION

Publisher

Iowa State University Digital Repository, Ames IA (United States)

Available for download on Tuesday, January 01, 2019

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