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@ARTICLE{Kintzel:20017,
author = {Kintzel, E.J. and Kidder, M.K. and Buchanan, A.C. and
Britt, P.F. and Mamontov, E. and Zamponi, M. and Herwig,
K.W.},
title = {{D}ynamics of 1,3-diphenylpropane tethered to the interior
pore surfaces of {MCM}-41},
journal = {The journal of physical chemistry / C},
volume = {116},
issn = {1932-7447},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PreJuSER-20017},
pages = {923 - 932},
year = {2012},
note = {A portion of this research was performed at Oak Ridge
National Laboratory's Spallation Neutron Source which is
sponsored by the Scientific User Facilities Division, Office
of Basic Energy Sciences, U.S. Department of Energy. M.K.K,
P.F.B., and A.C.B.III, acknowledge the support of the
Division of Chemical Sciences, Geosciences, and Biosciences,
Office of Basic Energy Sciences, U.S. Department of Energy.
We also acknowledge the support of the National Institute of
Standards and Technology, U.S. Department of Commerce, in
providing some of the neutron research facilities used in
this work. This work utilized facilities supported in part
by the National Science Foundation under Agreement No.
DMR-094477. We would like to acknowledge the assistance of
A.T. Ruffin in early data analysis and would like to thank
A. L. Chaffee for fruitful discussions and the kind use of
the images used in Figure 4.},
abstract = {The diffusive motions of covalently tethered
1,3-diphenylpropane (DPP) via a silyl-aryl-ether linkage in
the mesopores of MCM-41 were studied by quasielastic neutron
scattering. The geometric effect of pore radius was
investigated with samples having pores that ranged from 1.6
to 3.0 nm in diameter and highest achievable DPP grafting
density. The effect of molecular crowding was investigated
in 3.0 rim diameter pores for surface coverage ranging from
0.60 to 1.61 DPP/nm(2). Temperature dependence was
determined for large pore diameter samples from 240 to 370
K. As the DPP molecules remain attached over this entire
temperature range, data were analyzed in terms of a model of
localized diffusion inside a sphere. Only the motions of the
DPP hydrogen atoms were considered because of the high
sensitivity of neutron scattering to the presence of
hydrogen. As atoms far from the attachment point have a
greater range of motion than those nearer the tether, the
radius of the sphere limiting the motion of individual
hydrogen atoms was allowed to increase based on the atom's
distance from the tether point Both smaller pore diameters
and higher DPP grafting density resulted in larger amplitude
motion while the diffusion coefficient was greatest in the
largest pores at highest DPP density. These observations
support a model where the DPP molecules prefer an
orientation allowing close proximity to the MCM-41 pore
surface and are forced into the pore interior by either the
steric effect of small pore diameter or by increased
competition for surface area at high molecule surface
coverage.},
keywords = {J (WoSType)},
cin = {ICS-1 / JCNS (München) ; Jülich Centre for Neutron
Science JCNS (München) ; JCNS-FRM-II / JCNS-1},
ddc = {540},
cid = {I:(DE-Juel1)ICS-1-20110106 /
I:(DE-Juel1)JCNS-FRM-II-20110218 /
I:(DE-Juel1)JCNS-1-20110106},
pnm = {BioSoft: Makromolekulare Systeme und biologische
Informationsverarbeitung / Großgeräte für die Forschung
mit Photonen, Neutronen und Ionen (PNI)},
pid = {G:(DE-Juel1)FUEK505 / G:(DE-Juel1)FUEK415},
experiment = {EXP:(DE-MLZ)External-20140101},
shelfmark = {Chemistry, Physical / Nanoscience $\&$ Nanotechnology /
Materials Science, Multidisciplinary},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000298978700113},
doi = {10.1021/jp209458a},
url = {https://juser.fz-juelich.de/record/20017},
}