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polyelectrolyte multilayers in Capillary Electrophoresis

CHEMPLUSCHEM 2022年第4期87卷 e202200028-e202200028页

作者： Roca, Sebastien Dhellemmes, Laura Leclercq, Laurent Cottet, Herve Univ Montpellier IBMM CNRS ENSCM Montpellier France

Capillary electrophoresis (CE) has been proven to be a performant analytical method to analyze both small and macro molecules. Indeed, it is capable of separating compounds of the same nature according to differences in their charge to size ratios, particularly proteins, monoclonal antibodies and peptides. However, one of the major obstacles to reach high separation efficiency remains the adsorption of solutes on the capillary wall. Among the different coating approaches used to control and minimize solute adsorption, polyelectrolyte multilayers can be applied to CE as a versatile approach. These coatings are made up of alternating layers of polycations and polyanions, and may be used in acidic, neutral or basic conditions depending on the solutes to be analyzed. This Review provides an overview of Successive Multiple Ionic-polymer Layer (SMIL) coatings used in CE, looking at how different parameters induce variations on the electro-osmotic flow (EOF), separation efficiency and coating stability, as well as their promising applications in the biopharmaceutical field.

关键词： electro-osmotic flow electrophoresis polyelectrolyte multilayers proteins separation efficiency

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Biocompatible polyelectrolyte multilayers with Copper Oxide and Zinc Oxide Nanoparticles for Inhibiting Bacterial Growth

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ACS APPLIED NANO MATERIALS 2024年第11期7卷 12550-12563页

作者： Mlinaric, Nives Matijakovic Altenried, Stefanie Selmani, Atida Nikolic, Juraj Ucakar, Aleksander Zore, Anamarija Abram, Anze Lehner, Sandro Skapin, Andrijana Sever Kuster, Monika Roblegg, Eva Kovacevic, Davor Ren, Qun Bohinc, Klemen Univ Ljubljana Fac Hlth Sci Ljubljana 1000 Slovenia Lab Biointerfaces Swiss Fed Labs Mat Sci & Technol Empa CH-9014 St Gallen Switzerland Karl Franzens Univ Graz Inst Pharmaceut Sci Pharmaceut Technol & Biopharm A-8010 Graz Austria Univ Zagreb Fac Sci Dept Chem Zagreb 10000 Croatia Jozef Stefan Inst Ljubljana 1000 Slovenia Slovenian Natl Bldg & Civil Engn Inst Ljubljana 1000 Slovenia

The prevalence of bacterial infections presents a significant challenge in the medical field, demanding effective strategies to impede bacterial adhesion and growth on various surfaces. The conducted study investigates the efficacy of polyelectrolyte multilayers & horbar;comprising poly(allylamine hydrochloride) (PAH) and alginate (ALG)& horbar;embedded with zinc oxide (ZnO) and copper oxide (CuO) nanoparticles (NPs) to inhibit bacterial adhesion on stainless-steel surfaces. Surface characterization involved zeta potential, contact angle, and roughness assessments. The effect of NP composition, size, and morphology in conjunction with polycation or polyanion terminating multilayers was evaluated against planktonic and surface-adhered Escherichia coli (E. coli) cells. Surfaces with the positively charged PAH-terminating multilayer displayed higher water contact angles (approximate to 63 degrees) than the negatively charged ALG-terminating multilayers (approximate to 45 degrees). multilayers containing ZnO NPs showed a significant inhibition of planktonic E. coli growth, >99%. Moreover, complete growth inhibition of surface-adhered E. coli was achieved for multilayers containing both ZnO and CuO. Due to their larger specific surface area, rod-like ZnO NPs displayed higher antibacterial activity. The samples with ALG as the terminating layer showed more substantial antibacterial properties than samples with PAH as the terminating layer. Biocompatibility tests on immortalized human keratinocyte cells revealed good compatibility with multilayers incorporating NPs. In summary, this study underscores the potential of ZnO and CuO NPs within PAH/ALG multilayers for antibacterial applications without compromising their cytocompatibility.

关键词： polyelectrolyte multilayers alginate poly(allylaminehydrochloride) CuO ZnO nanoparticles Escherichia coli

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Au@Ag Core-shell Nanorods Self-assembled on polyelectrolyte multilayers for Ultra-High Sensitivity SERS Fiber Probes

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Journal of Wuhan University of Technology(Materials Science) 2023年第3期38卷 505-513页

作者：王文博 XIONG Wenhao LONG Yuting 李宏 State Key Laboratory of Silicate Materials for Architectures Wuhan University of TechnologyWuhan 430070China School of Science School of Chip IndustryHubei University of TechnologyWuhan 430068China

We demonstrated a chemical process in the fabrication of a SERS fiber probe with an ultrahigh *** synthesis was carried out by preparing Au@Ag core-shell nanorods (Au@Ag-NRs) selfassembled on polyelectrolyte (PE) multilayers,for which Au@Ag-NRs were controlled by adjusting the silver layer *** effect of silver layer thickness of Au@Ag-NRs on the SERS performance of the fiber probe was *** SERS fiber probe shows the best performance when the silver layer thickness is controlled at 8.57 *** the condition of optimizing silver layer thickness,the fiber probe exhibits ultra-high sensitivity (i e,10^(-10) M crystalline violet,CV),good reproducibility (i e,RSD of 3.5%) and ***,electromagnetic field distribution of the SERS fiber probe was also *** strongest enhancement is found within the core of fiber,whereas a weakened electromagnetic field exists in the fiber cladding *** SERS fiber probe can be a good candidate in ultra-trace detection for biomedical and environmental areas.

关键词： surface-enhanced Raman scattering(SERS) optical fiber probe self-assembly Au@Ag core-shell nanorods(Au@Ag-NRs) polyelectrolyte multilayers

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Bioinspired nanostructured hydroxyapatite-polyelectrolyte multilayers for stone conservation

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JOURNAL OF COLLOID AND INTERFACE SCIENCE 2024年 674卷 459-473页

作者： Hafez, Iosif T. Biskos, George Cyprus Inst Sci & Technol Archaeol & Culture Res Ctr CY-2121 Nicosia Cyprus Cyprus Inst Climate & Atmosphere Res Ctr CY-2121 Nicosia Cyprus Delft Univ Technol Fac Civil Engn & Geosci NL-2628 CN Delft Netherlands

Stone-built cultural heritage faces threats from natural forces and anthropogenic pollutants, including local climate, acid rain, and outdoor conditions like temperature fluctuations and wind exposure, all of which impact their structural integrity and lead to their degradation. The development of a water-based, environmentallyfriendly protective coatings that meet a combination of requirements posed by the diversity of the substrates, different environmental conditions, and structures with complex geometries remains a formidable challenge, given the numerous obstacles faced by current conservation strategies. Here we report the structural, electrical, and mechanical characterization, along with performance testing, of a nanostructured hydrophilic and selfhealing hybrid coating based on hydroxyapatite (HAp) nanocrystals and polyelectrolyte multilayers (PEM), formed in-situ on Greek marble through a simple spray layer-by-layer surface functionalization technique. The polyelectrolyte-hydroxyapatite multilayer (PHM) structure resembled the design of naturally forming trabecular bone, attained at a short procedural time. It exhibited chemical affinity, aesthetical compatibility and resistance to weathering while offering reversibility. The proposed method is able to generate micron-sized coatings with controlled properties, such as adhesion and self-healing, leading to less weathered surfaces. Our results show that the PHM is a highly effective protective material that can be applied for stone protection and other similar applications.

关键词： Stone protection Hybrid coatings Hydroxyapatite polyelectrolyte multilayers Self -healing

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Memristive Effect in Ti3C2Tx (MXene) polyelectrolyte multilayers

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CHEMPHYSCHEM 2023年第17期24卷 e202300187-e202300187页

作者： Aglikov, Aleksandr Volkova, Olga Bondar, Anna Moskalenko, Ivan Novikov, Alexander Skorb, Ekaterina V. Smirnov, Evgeny ITMO Univ Infochem Sci Ctr Lomonosova str 9 St Petersburg 191002 Russia

The emerging novel class of two-dimensional materials - MXenes - have attracted significant research attention. However, there are only few reports on using the most prominent member of the MXene family, Ti3C2Tx, as an active material for memristive devices within a polyelectrolyte matrix and its deposition on inert electrodes like ITO and Pt. In this study, we systematically investigate Ti3C2Tx MXenes synthesized with two classical delamination agents, such as lithium chloride and tetramethylammonium hydroxide, to identify the most suitable candidate for memristive device applications. The characteristics of memristors based on the hybrid structures consisting of MXene-polyelectrolyte multilayers, specifically polyethyleneimine (PEI) and poly(sodium 4-styrenesulfonate) (PSS) are explored. The PEI(MXene)/PSS memristor exhibits a voltage threshold (V-SET/RESET) range of 1.5-2.0 V, enabling the transition from a high-resistive state (HRS) to a low-resistive state (LRS), along with a significant current switching ratio of approximately two orders of magnitude. The observed V-SET/RESET difference of approximately 4 V is further supported by density functional theory (DFT) calculated redox potential. These findings underscore the potential of polyelectrolyte-based memristors, such as the in PEI-Ti3C2Tx-PSS system, in facilitating the development of highly functional, self-assembled memristive devices with diverse applications.

关键词： DFT memristive effect MXene polyelectrolyte multilayers self-assembly

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Specific Ion Effects of Divalent Cations on the Formation and Properties of polyelectrolyte multilayers

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CHEMISTRYSELECT 2025年第12期10卷

作者： Mesic, Mia Klacic, Tin Kovacvevic, Davor Univ Zagreb Fac Sci Dept Chem Div Phys Chem Horvatovac 102A Zagreb 10000 Croatia Rudjer Boskovic Inst Div Mat Chem Bijenicka Cesta 54 Zagreb 10000 Croatia

Multilayer films made of strong polyelectrolytes poly(diallyldimethylammonium chloride) and poly(sodium 4-styrenesulfonate) were built-up on silicon wafer using the layer-by-layer method. The films were built-up in the presence of various divalent cations (Mg2+, Ca2+, Sr2+, Ni2+, Zn2+, and Cu2+) to examine how the nature of cations affects the properties of the film. The results have shown that the thickness, morphology, and roughness of films prepared in the presence of transition metal cations are not significantly different. In contrast, these properties varied for multilayers prepared in the presence of alkaline earth metal cations. The difference in the ion-specific behavior of these two classes of cations was explained by the difference in the hydration of these ions and by the bridging of polyelectrolyte chains with ions. While transition metal cations have similar hydration parameters, alkaline earth cations have different degrees of hydration and a better ability to form bridging bonds with polyelectrolyte monomers.

关键词： Divalent cations polyelectrolyte multilayers polyelectrolytes Specific ion effects

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Enhanced monovalent over divalent cation selectivity with polyelectrolyte multilayers in membrane capacitive deionization via optimization of operational conditions

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DESALINATION 2022年 522卷 115391-115391页

作者： Sahin, Sevil Zuilhof, Han Zornitta, Rafael L. de Smet, Louis C. P. M. Wageningen Univ Lab Organ Chem Stippeneng 4 NL-6708 WE Wageningen Netherlands

In this work, we tuned the ion selectivity of a polyelectrolyte multilayer (PEM)-coated, cation-exchange membrane (CMX) in a membrane capacitive deionization (MCDI) process by carefully studying different operational modes, namely constant voltage (CV) and constant current (CC). The monovalent cation selectivity and its time dependent behavior were monitored at different voltage and current values. Upon optimizing the current density (10 A/m(2)) and the number of polyelectrolyte bilayers (5.5) on the CMX membranes, a time-independent and nearly full monovalent cation selectivity was obtained for various feed solutions, provided a polycationterminated PEM was applied. Furthermore, the selectivity values of several commercially available cation exchange membranes were tested under the optimized conditions and compared with CMX and PEM-CMX, yielding the best performance for PEM-CMX, regardless the composition of feed solution. Before this optimization, this MCDI system showed a time-dependent selectivity, with a maximum of rho Mg-Na approximate to 3. The results were rationalized by applying an MCDI model based on the dynamic potential profile, describing the potential drops across the membrane and demonstrating a threshold for the current density.

关键词： Cation selectivity polyelectrolyte multilayers Capacitive deionization Ion-exchange membrane Ion separation

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Polarity studies of single polyelectrolyte layers in polyelectrolyte multilayers probed by steady state and life time doxorubicin fluorescence

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JOURNAL OF COLLOID AND INTERFACE SCIENCE 2022年第Part1期607卷 153-162页

作者： Martinelli, Hernan Tasca, Elisamaria Andreozzi, Patrizia Libertone, Sara Ritacco, Hernan Giustini, Mauro Moya, Sergio E. Inst Fis Sur IFISUR CONICET Av Alem 1253 RA-8000 Bahia Blanca Buenos Aires Argentina Basque Res & Technol Alliance BRTA CIC BiomaGUNE Soft Matter Nanotechnol Grp Paseo Miramon 182 San Sebastian 20014 Guipazcoa Spain Univ Roma La Sapienza Chem Dept Ple Aldo Moro 5 I-00185 Rome Italy Univ Florence Dept Chem Ugo Schiff Consorzio Sistemi Grande Interfase Via Lastruccia 3 I-50019 Sesto Fiorentino FI Italy

Hypothesis: Polarity in polyelectrolyte multilayers (PEMs) may vary from the inner to the top layers of the film as the charge compensation of the layers is more effective inside the PEMs than in outer layers. Doxorubicin hydrochloride (DX) is used here to sense polarity at the single polyelectrolyte level inside PEMS. Experimental: DX is complexed electrostatically to a polyanion, either polystyrene sulfonate (PSS) or polyacrylic acid (PAA) and assembled at selected positions in a multilayer of the polyanion and polyallylamine hydrochloride (PAH) as polycation. Local polarity in the layer domain is evaluated through changes in the intensity ratio of the first to second band of spectra of DX (I1/I2 ratio) by steady state fluorescence, and by Lifetime fluorescence. Findings: PAH/PSS multilayers, show a polarity similar to water with DX/PSS as top layer, decreasing to I1/ I2 ratios similar to organic solvents as the number of polyelectrolyte layers assembled on top increases. For PAH/PAA multilayers, polarity values reflect a more polar environment than water when DX/PAA is the top layer, remaining unaltered by the assembly of polyelectrolyte layers on top. Results show that different polar environments may be present in a PEM when considering polarity at the single layer level. (c) 2021 Published by Elsevier Inc.

关键词： Polarity Doxorubicin Fluorescence Lifetime polyelectrolyte multilayers Layer by Layer Technique

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Heteroaggregation between particles modified by polyelectrolyte multilayers

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS 2022年第0期650卷

作者： Cerbelaud, Manuella Bennani, Yasmine Peyratout, Claire Univ Limoges CNRS IRCER UMR 7315 F-87000 Limoges France

The heteroaggregation of particles is interesting in many fields and particularly in the field of ceramic shaping. In general, heteroaggregation is obtained by mixing powders with opposite surface charges, which may require in some cases surface modifications of the particles. Here we propose to study the behavior of suspensions composed of a mixture of particles with positive and negative charges, created by the adsorption of poly -electrolyte multilayers on their surface. Particular attention is paid to the effect of the number of layers of adsorbed polyelectrolytes and of the ionic strength. This study shows that these surface modifications allow, whatever the number of layers, to have heteroaggregation in the absence of salt. Moreover, depending on the number of adsorbed layers, the addition of salt has a different effect on the suspension behavior. These phe-nomena can be explained by screening effects already mentioned in the literature for unmixed suspensions of particles modified by polyelectrolyte multilayers. As a consequence, this study highlights that the study of heteroaggregation in these systems is a very simple way to analyze this effect of screening which is difficult to observe on non-mixed suspensions.

关键词： Heteroaggregation Colloid surface modifications polyelectrolyte multilayers Salt effect

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Simultaneous, monovalent ion selectivity with polyelectrolyte multilayers and intercalation electrodes in capacitive deionization

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CHEMICAL ENGINEERING JOURNAL 2022年 432卷 128329-128329页

作者： Singh, K. Sahin, S. Gamaethiralalage, J. G. Zornitta, Rafael L. de Smet, L. C. P. M. Wageningen Univ Lab Organ Chem Stippeneng 4 NL-6708 WE Wageningen Netherlands Wetsus European Ctr Excellence Sustainable Water Technol Oostergoweg 9 NL-8911 MA Leeuwarden Netherlands

Selective ion separation via capacitive deionization (CDI) is of relevance because of its environmental and in-dustrial applications in water purification and softening, heavy metal removal, and resource recovery. Conventionally, carbon electrodes and ion-selective membranes have been used for selective removal of anions and cations. In this study, we engineered a CDI cell with two identical NiHCF electrodes, separated by an anion-exchange membrane coated with a polyelectrolyte multilayer (PEM), for simultaneous and selective separation of monovalent over divalent anions and cations. The modified membrane rejects divalent over monovalent anions while the NiHCF electrodes selectively adsorb monovalent over divalent ions. A separation factor (beta) of 7 < beta < 14 was obtained for Cl- over SO42-, while an average beta of & AP;17 was obtained for Na+ over Mg2+, reflecting the preference of the modified membrane and the electrodes, respectively. Moreover, this preference was preserved at low concentrations of monovalent ions as well. This tandem use of intercalation electrodes and a PEM membrane provides a new and facile method for simultaneous cation and anion selectivity in CDI, opening new avenues for enhanced and tunable separations from complex ion mixtures

关键词： Ion selectivity polyelectrolyte multilayers Prussian blue analogues Capacitive deionization

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