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Short versus long chain polyelectrolyte multilayers: a direct comparison of self-assembly and structural properties

  • Successful layer-by-layer (LbL) growth of short chain (similar to 30 repeat units per chain) poly(sodium styrene sulfonate) (PSS)-poly(diallyl dimethylammonium chloride) (PDADMAC) multilayers is presented for the first time and compared with the growth of equivalent long chain polyelectrolyte multilayers (PEMs). A detailed study performed by quartz crystal microbalance with dissipation (QCM-D) is carried out and three main processes are identified: (i) initial mass uptake, (ii) adsorption desorption during layer equilibration and (iii) desorption during rinsing. In contrast to the high stability and strong layer increment of high molecular weight (HMW) PEMs, layer degradation characterizes low molecular weight (LMW) multilayers. In particular, two different instability phenomena are observed: a constant decrease of sensed mass during equilibration after PDADMAC adsorption, and a strong mass toss by salt-free rinsing after PSS adsorption. Yet, an increase of salt concentration leads to much stronger layer growth. First, when theSuccessful layer-by-layer (LbL) growth of short chain (similar to 30 repeat units per chain) poly(sodium styrene sulfonate) (PSS)-poly(diallyl dimethylammonium chloride) (PDADMAC) multilayers is presented for the first time and compared with the growth of equivalent long chain polyelectrolyte multilayers (PEMs). A detailed study performed by quartz crystal microbalance with dissipation (QCM-D) is carried out and three main processes are identified: (i) initial mass uptake, (ii) adsorption desorption during layer equilibration and (iii) desorption during rinsing. In contrast to the high stability and strong layer increment of high molecular weight (HMW) PEMs, layer degradation characterizes low molecular weight (LMW) multilayers. In particular, two different instability phenomena are observed: a constant decrease of sensed mass during equilibration after PDADMAC adsorption, and a strong mass toss by salt-free rinsing after PSS adsorption. Yet, an increase of salt concentration leads to much stronger layer growth. First, when the rinsing medium is changed from pure water to 0.1 M NaCl, the mass loss during rinsing is reduced, irrespective of molecular weight. Second, an increase in salt concentration in the LMW PE solutions causes a larger increment during the initial adsorption step, with no effect on the rinsing. Finally, the mechanical properties of the two systems are extracted from the measured frequency and dissipation shifts, as they offer a deeper insight into the multilayer structures depending on chain length and outermost layer. The paper enriches the field of PE assembly by presenting the use of very short PE chains to form multilayers and elucidates the role of preparation conditions to overcome the limitation of layer stability.show moreshow less

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Metadaten
Author:Samantha Micciulla, Samuel Dodoo, Chloe Chevigny, André LaschewskyORCiDGND, Regine von KlitzingORCiD
DOI:https://doi.org/10.1039/c4cp03439b
ISSN:1463-9076 (print)
ISSN:1463-9084 (online)
Pubmed Id:http://www.ncbi.nlm.nih.gov/pubmed?term=25205523
Parent Title (English):Physical chemistry, chemical physics : a journal of European Chemical Societies
Publisher:Royal Society of Chemistry
Place of publication:Cambridge
Document Type:Article
Language:English
Year of first Publication:2014
Year of Completion:2014
Release Date:2017/03/27
Volume:16
Issue:40
Pagenumber:11
First Page:21988
Last Page:21998
Funder:Deutsche Forschungsgenzeinschaft DPG [SPP 1369]
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie
Peer Review:Referiert