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@ARTICLE{Prevost:18193,
author = {Prevost, S. and Riemer, S. and Fischer, W. and Haag, R. and
Böttcher, C. and Gummel, J. and Grillo, I. and Appavou,
M.-S. and Gradzielski, M.},
title = {{C}olloidal {S}tructure and {S}tability of
{DNA}/{P}olycations {P}olyplexes investigated by {S}mall
{A}ngle {S}cattering},
journal = {Biomacromolecules},
volume = {12},
issn = {1525-7797},
address = {Columbus, Ohio},
publisher = {American Chemical Soc.},
reportid = {PreJuSER-18193},
pages = {4272},
year = {2011},
note = {For allocation of SANS and SAXS beam times, we are grateful
to the HZB, ILL, JCNS, and ESRF. For help with the
scattering experiments, we would like to thank T. Narayanan
(ESRF, ID2). For her constant help during the SANS and SAXS
measurements, we are indebted to P. Heunemann. N. Graeber
and A. Walther are thanked for preparation of samples. SANS
experiments at the HZB and JCNS have been supported by the
European Commission under the 7th Framework Program through
the Key Action: Strengthening the European Research Area,
Research Infrastructures, Contract No. 226 507 (NMI3). The
research project has been supported and funded by the SFB
448 of the Deutsche Forschungsgemeinschaft.},
abstract = {Polyplexes of short DNA-fragments (300 b.p., 100 nm) with
tailor-made amine-based polycations of different
architectures (linear and hyperbranched) were investigated
in buffer solution as a function of the mixing ratio with
DNA. The resulting dispersed polyplexes were characterized
using small-angle neutron and X-ray scattering (SANS, SAXS)
as well as cryo-TEM with respect to their mesoscopic
structure and their colloidal stability. The linear
polyimines form rather compact structures that have a high
tendency for precipitation. In contrast, the hyperbranched
polycation with enzymatic-labile pentaethylenehexamine arms
(PEHA) yields polyplexes colloidally stable for months. Here
the polycation coating of DNA results in a homogeneous
dispersion based on a fractal network with low structural
organization at low polycation amount. With increasing
polycation, bundles of tens of aligned DNA rods appear that
are interconnected in a fractal network with a typical
correlation distance on the order of 100 nm, the average
length of the DNA used. With higher organization comes a
decrease in stability. The 3D network built by these beams
can still exhibit some stability as long as the material
concentration is large enough, but the structure collapses
upon dilution. SAXS shows that the complexation does not
affect the local DNA structure. Interestingly, the
structural findings on the DNA polyplexes apparently
correlate with the transfection efficiency of corresponding
siRNA complexes. In general, these finding not only show
systematic trends for the colloid stability, but may allow
for rational approaches to design effective transfection
carriers.},
keywords = {Colloids: chemistry / DNA: chemistry / DNA: metabolism /
DNA: ultrastructure / Polyamines: chemistry / Polymers:
chemistry / Scattering, Small Angle / Colloids (NLM
Chemicals) / Polyamines (NLM Chemicals) / Polymers (NLM
Chemicals) / polycations (NLM Chemicals) /
pentaethylenehexamine (NLM Chemicals) / DNA (NLM Chemicals)
/ J (WoSType)},
cin = {ICS-1 / JCNS (München) ; Jülich Centre for Neutron
Science JCNS (München) ; JCNS-FRM-II / JCNS-1 / JCNS-2},
ddc = {540},
cid = {I:(DE-Juel1)ICS-1-20110106 /
I:(DE-Juel1)JCNS-FRM-II-20110218 /
I:(DE-Juel1)JCNS-1-20110106 / I:(DE-Juel1)JCNS-2-20110106},
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)KWS2-20140101},
shelfmark = {Biochemistry $\&$ Molecular Biology / Chemistry, Organic /
Polymer Science},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:22074384},
UT = {WOS:000297782100013},
doi = {10.1021/bm201184w},
url = {https://juser.fz-juelich.de/record/18193},
}