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Colloids and Polymers: An Issue in Honor of Professor Björn Lindman

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Physical Chemistry".

Deadline for manuscript submissions: closed (30 September 2023) | Viewed by 14731

Special Issue Editors

Dr. Artur Valente

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Guest Editor
Department of Chemistry, University of Coimbra, 3004-535 Coimbra, Portugal
Interests: transport phenomena; surfactants; biopolymers; polysaccharides; supramolecular chemistry
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Mariette M. Pereira

E-Mail Website
Guest Editor
Department of Chemistry, University of Coimbra, Coimbra, Portugal
Interests: organic synthesis; CO2-based polymeric materials; medicinal chemistry; sustained catalytic processes
Special Issues, Collections and Topics in MDPI journals
Prof. Dr. Alberto Pais

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Guest Editor
Department of Chemistry, University of Coimbra, Coimbra, Portugal
Interests: molecular simulation; polymers; polyelectrolytes; computational chemistry; delivery systems
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

This Special Issue of Molecules is dedicated to Professor Björn Lindman on the occasion of his 80th birthday.

Björn Lindman received a Chemical Engineering degree from the Royal Institute of Technology, Stockholm, in 1966. In 1971, Björn defended his PhD thesis at Lund University. In 1971 he became a Lecturer (Associate Professor) in the Physical Chemistry Department and in 1978 he achieved the position of Chair Professor in the Division of Physical Chemistry 1, Department of Chemistry and Chemical Engineering at Lund University. In 1998, he was appointed Professor of the Department of Chemistry of the University of Coimbra, and since 2013 has been a Visiting Professor at Nanyang Technical University, Singapore. He was Guest Professor at MidSweden Univ., Sundsvall, Sweden from 2014 to 2019. His work has been recognized with many awards, including the Unilever Award, Royal Institute of Technology; Arrhenius Award of the Swedish Chemical Society; Langmuir Award—ACS; Bror Holmberg Medal, Swedish Chemical Society; Overbeek Gold Medal of the European Colloid and Interface Society; and Lifetime Achievement Award of the International Association of Colloid and Interface Scientists in 2015. He is a Fellow of the Royal Swedish Academy of Sciences and a Fellow of the Royal Swedish Academy of Engineering Sciences.

Björn published his first paper in 1968 on the nuclear quadrupole relaxation of quaternary ammonium bromides. He then paved the way for the use of NMR self-diffusion in the characterization of self-assembly in colloidal multicomponent systems. He was also the first to quantitatively interpret the experimental self-diffusion coefficients of multicomponent systems and their dependence on the diffusion coefficients of each species and corresponding mole fraction. This quantitative relationship is known as Lindman’s law. In addition, Björn has made seminal contributions in areas involving ion binding, surfactants and polymer–surfactant systems. In the last 15 years, Björn has also been pivotal in the interpretation of the cellulose dissolution phenomena in different solvents, including water, by highlighting the role of intermolecular hydrophobic interactions. This contribution demonstrates Björn’s restless spirit, and how he is always ready for new scientific challenges, presenting major contributions for the development of science.

In his academic and scientific career, Björn’s ability to attract doctoral students (he has supervised over 40 PhD theses) and to establish collaborations with researchers around the world is also worthy of mention. He concluded very early on that science is a collective design and that discussion and collaborations are the most effective way to reach the proposed goals. Thus, he was one of the founders of the European Colloid and Interface Society. 

We plan to organize a Special Issue honoring Björn Lindman’s distinguished scientific career over the past 60 years and his 80th birthday. This Special Issue will consist of communications, original research articles, and review articles related to colloidal systems and polymers—two of Björn’s major interests.

Dr. Artur Valente
Prof. Dr. Mariette M. Pereira
Prof. Dr. Alberto Pais
Guest Editors

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Keywords

  • colloidal systems
  • polymers
  • cellulose
  • surfactants
  • polyelectrolytes

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Published Papers (7 papers)

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Research

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18 pages, 2685 KiB  
Article
Phase Behavior and Structure of Poloxamer Block Copolymers in Protic and Aprotic Ionic Liquids
by Aikaterini Tsoutsoura, Zhiqi He and Paschalis Alexandridis
Molecules 2023, 28(21), 7434; https://doi.org/10.3390/molecules28217434 - 5 Nov 2023
Cited by 3 | Viewed by 1971
Abstract
Ionic liquids are promising media for self-assembling block copolymers in applications such as energy storage. A robust design of block copolymer formulations in ionic liquids requires fundamental knowledge of their self-organization at the nanoscale. To this end, here, we focus on modeling two-component [...] Read more.
Ionic liquids are promising media for self-assembling block copolymers in applications such as energy storage. A robust design of block copolymer formulations in ionic liquids requires fundamental knowledge of their self-organization at the nanoscale. To this end, here, we focus on modeling two-component systems comprising a Poly(ethylene oxide)-poly (propylene oxide)-Poly(ethylene oxide) (PEO-PPO-PEO) block copolymer (Pluronic P105: EO37PO58EO37) and room temperature ionic liquids (RTILs): protic ethylammonium nitrate (EAN), aprotic ionic liquids (1-butyl-3-methylimidazolium hexafluorophosphate (BMIMPF6), or 1-butyl-3-methylimidazolium tetrafluoroborate (BMIMBF4). Rich structural polymorphism was exhibited, including phases of micellar (sphere) cubic, hexagonal (cylinder), bicontinuous cubic, and lamellar (bilayer) lyotropic liquid crystalline (LLC) ordered structures in addition to solution regions. The characteristic scales of the structural lengths were obtained using small-angle X-ray scattering (SAXS) data analysis. On the basis of phase behavior and structure, the effects of the ionic liquid solvent on block copolymer organization were assessed and contrasted to those of molecular solvents, such as water and formamide. Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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13 pages, 3163 KiB  
Article
Luminescent Papers with Asymmetric Complexes of Eu(III) and Tb(III) in Polymeric Matrices and Suggested Combinations for Color Tuning
by Roberto J. Aguado, Beatriz O. Gomes, Luisa Durães and Artur J. M. Valente
Molecules 2023, 28(16), 6164; https://doi.org/10.3390/molecules28166164 - 21 Aug 2023
Cited by 5 | Viewed by 1590
Abstract
Complexes of lanthanide ions, such as Eu(III) (red light emission) and Tb(III) (green light emission), with proper ligands can be highly luminescent and color-tunable, also attaining yellow and orange emission under UV radiation. The ligands employed in this work were poly(sodium acrylate), working [...] Read more.
Complexes of lanthanide ions, such as Eu(III) (red light emission) and Tb(III) (green light emission), with proper ligands can be highly luminescent and color-tunable, also attaining yellow and orange emission under UV radiation. The ligands employed in this work were poly(sodium acrylate), working as polymeric matrix, and 1,10-phenanthroline, taking advantage of its antenna effect. Possibilities of color display were further enhanced by incorporating a cationic polyfluorene with blue emission. This strategy allowed for obtaining cyan and magenta, besides the aforementioned colors. Uncoated cellulose paper was impregnated with the resulting luminescent inks, observing a strong hypsochromic shift in excitation wavelength upon drying. Hence, while a cheap UV-A lamp sufficed to reveal the polyfluorene’s blue emission, shorter wavelengths were necessary to visualize the emission due to lanthanide ions as well. The capacity to reveal, with UV-C radiation, a full-color image that remains invisible under natural light is undoubtedly useful for anti-counterfeiting applications. Furthermore, both lanthanide ion complexes and polyfluorenes were shown to have their luminescence quenched by Cu(II) ions and nitroarenes, respectively. Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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19 pages, 3954 KiB  
Article
Interactions between Ionic Cellulose Derivatives Recycled from Textile Wastes and Surfactants: Interfacial, Aggregation and Wettability Studies
by Catarina Costa, André Viana, Isabel S. Oliveira and Eduardo F. Marques
Molecules 2023, 28(8), 3454; https://doi.org/10.3390/molecules28083454 - 13 Apr 2023
Cited by 4 | Viewed by 1836
Abstract
Interactions between polymers (P) and surfactants (S) in aqueous solution lead to interfacial and aggregation phenomena that are not only of great interest in physical chemistry but also important for many industrial applications, such as the development of detergents and fabric softeners. Here, [...] Read more.
Interactions between polymers (P) and surfactants (S) in aqueous solution lead to interfacial and aggregation phenomena that are not only of great interest in physical chemistry but also important for many industrial applications, such as the development of detergents and fabric softeners. Here, we synthesized two ionic derivatives—sodium carboxymethylcellulose (NaCMC) and quaternized cellulose (QC)—from cellulose recycled from textile wastes and then explored the interactions of these polymers with assorted surfactants—cationic (CTAB, gemini), anionic (SDS, SDBS) and nonionic (TX-100)—commonly used in the textile industry. We obtained surface tension curves of the P/S mixtures by fixing the polymer concentration and then increasing the surfactant concentration. In mixtures where polymer and surfactant are oppositely charged (P−/S+ and P+/S−), a strong association is observed, and from the surface tension curves, we determined the critical aggregation concentration (cac) and critical micelle concentration in the presence of polymer (cmcp). For mixtures of similar charge (P+/S+ and P−/S−), virtually no interactions are observed, with the notable exception of the QC/CTAB system, which is much more surface active than the neat CTAB. We further investigated the effect of oppositely charged P/S mixtures on hydrophilicity by measuring the contact angles of aqueous droplets on a hydrophobic textile substrate. Significantly, both P−/S+ and P+/S− systems greatly enhance the hydrophilicity of the substrate at much lower surfactant concentrations than the surfactant alone (in particular in the QC/SDBS and QC/SDS systems). Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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16 pages, 3693 KiB  
Article
Assessing the Contribution of the Neutral Blocks in DNA/Block-Copolymer Polyplexes: Poly(acrylamide) vs. Poly(ethylene Oxide)
by Renata Mello Giona, Letícia Vitorazi and Watson Loh
Molecules 2023, 28(1), 398; https://doi.org/10.3390/molecules28010398 - 3 Jan 2023
Cited by 2 | Viewed by 1512
Abstract
The interaction of DNA with different block copolymers, namely poly (trimethylammonium chloride methacryloyoxy)ethyl)-block-poly(acrylamide), i.e., (PTEA)-b-(PAm), and poly (trimethylammonium chloride methacryloyoxy)ethyl)-block-poly(ethylene oxide), i.e., (PTEA)-b-(PEO), was studied. The nature of the cationic block was maintained fixed (PTEA), whereas the neutral blocks [...] Read more.
The interaction of DNA with different block copolymers, namely poly (trimethylammonium chloride methacryloyoxy)ethyl)-block-poly(acrylamide), i.e., (PTEA)-b-(PAm), and poly (trimethylammonium chloride methacryloyoxy)ethyl)-block-poly(ethylene oxide), i.e., (PTEA)-b-(PEO), was studied. The nature of the cationic block was maintained fixed (PTEA), whereas the neutral blocks contained varying amounts of acrylamide or (ethylene oxide) units. According to results from isothermal titration microcalorimetry measurements, the copolymers interaction with DNA is endothermic with an enthalpy around 4.0 kJ mol−1 of charges for (PTEA)-b-(PAm) and 5.5 kJ mol−1 of charges for (PTEA)-b-(PEO). The hydrodynamic diameters of (PTEA)-b-(PEO)/DNA and (PTEA)-b-(PAm)/DNA polyplexes prepared by titration were around 200 nm at charge ratio (Z+/−) < 1. At Z+/− close and above 1, the (PTEA)50-b-(PAm)50/DNA and (PTEA)50-b-(PAm)200/DNA polyplexes precipitated. Interestingly, (PTEA)50-b-(PAm)1000/DNA polyplexes remained with a size of around 300 nm even after charge neutralization, probably due to the size of the neutral block. Conversely, for (PTEA)96-b-(PEO)100/DNA polyplexes, the size distribution was broad, indicating a more heterogeneous system. Polyplexes were also prepared by direct mixture at Z+/− of 2.0, and they displayed diameters around 120–150 nm, remaining stable for more than 10 days. Direct and reverse titration experiments showed that the order of addition affects both the size and charge of the resulting polyplexes. Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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13 pages, 2011 KiB  
Article
Expanding the Toolbox for Bicelle-Forming Surfactant–Lipid Mixtures
by Rita Del Giudice, Nicolò Paracini, Tomas Laursen, Clement Blanchet, Felix Roosen-Runge and Marité Cárdenas
Molecules 2022, 27(21), 7628; https://doi.org/10.3390/molecules27217628 - 7 Nov 2022
Cited by 4 | Viewed by 2300
Abstract
Bicelles are disk-shaped models of cellular membranes used to study lipid–protein interactions, as well as for structural and functional studies on transmembrane proteins. One challenge for the incorporation of transmembrane proteins in bicelles is the limited range of detergent and lipid combinations available [...] Read more.
Bicelles are disk-shaped models of cellular membranes used to study lipid–protein interactions, as well as for structural and functional studies on transmembrane proteins. One challenge for the incorporation of transmembrane proteins in bicelles is the limited range of detergent and lipid combinations available for the successful reconstitution of proteins in model membranes. This is important, as the function and stability of transmembrane proteins are very closely linked to the detergents used for their purification and to the lipids that the proteins are embedded in. Here, we expand the toolkit of lipid and detergent combinations that allow the formation of stable bicelles. We use a combination of dynamic light scattering, small-angle X-ray scattering and cryogenic electron microscopy to perform a systematic sample characterization, thus providing a set of conditions under which bicelles can be successfully formed. Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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19 pages, 4723 KiB  
Article
A Semi-Empirical Model to Estimate Maximum Floc Size in a Turbulent Flow
by Mohamed Bizi
Molecules 2022, 27(17), 5550; https://doi.org/10.3390/molecules27175550 - 29 Aug 2022
Viewed by 1577
Abstract
The basic model for agglomerate breakage under the effect of hydrodynamic stress (dmax = C.G−γ) is only applicable for low velocity gradients (<500 s−1) and is often used for shear rates that are not representative of the [...] Read more.
The basic model for agglomerate breakage under the effect of hydrodynamic stress (dmax = C.G−γ) is only applicable for low velocity gradients (<500 s−1) and is often used for shear rates that are not representative of the global phenomenon. This paper presents a semi-empirical model that is able to predict mean floc size in a very broad shear range spanning from aggregation to floc fragmentation. Theoretical details and modifications relating to the orthokinetic flocculation output are also provided. Modelling changes in turbidity in relation to the velocity gradient with this model offer a mechanistic approach and provide kinetic agglomeration and breakage index ka and kb. The floc breakage mode is described by the relationship between the floc size and the Kolmogorov microscale. Shear-related floc restructuring is analysed by monitoring the fractal dimension. These models, as well as those used to determine floc porosity, density and volume fraction, are validated by the experimental results obtained from several flocculation operations conducted on ultrafine kaolin in a 4-litre reactor tank compliant with laws of geometric similarity. The velocity gradient range explored was from 60 to 6000 s−1. Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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Review

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30 pages, 11482 KiB  
Review
Perspectives on the Lindman Hypothesis and Cellulose Interactions
by Magnus Norgren, Carolina Costa, Luís Alves, Alireza Eivazi, Christina Dahlström, Ida Svanedal, Håkan Edlund and Bruno Medronho
Molecules 2023, 28(10), 4216; https://doi.org/10.3390/molecules28104216 - 21 May 2023
Cited by 10 | Viewed by 2995
Abstract
In the history of cellulose chemistry, hydrogen bonding has been the predominant explanation when discussing intermolecular interactions between cellulose polymers. This is the general consensus in scholarly textbooks and in many research articles, and it applies to several other biomacromolecules’ interactions as well. [...] Read more.
In the history of cellulose chemistry, hydrogen bonding has been the predominant explanation when discussing intermolecular interactions between cellulose polymers. This is the general consensus in scholarly textbooks and in many research articles, and it applies to several other biomacromolecules’ interactions as well. This rather unbalanced description of cellulose has likely impacted the development of materials based on the processing of cellulose—for example, via dissolution in various solvent systems and regeneration into solid materials, such as films and fibers, and even traditional wood fiber handling and papermaking. In this review, we take as a starting point the questioning of the general description of the nature of cellulose and cellulose interactions initiated by Professor Björn Lindman, based on generic physicochemical reasoning about surfactants and polymers. This dispute, which became known as “the Lindman hypothesis”, highlights the importance of hydrophobic interactions in cellulose systems and that cellulose is an amphiphilic polymer. This paper elaborates on Björn Lindman’s contribution to the subject, which has caused the scientific community to revisit cellulose and reconsider certain phenomena from other perspectives. Full article
(This article belongs to the Special Issue Colloids and Polymers: An Issue in Honor of Professor Björn Lindman)
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