The role of pore size and mechanical properties on the accumulation, retention and distribution of F98 glioblastoma cells in macroporous hydrogels.

Glioblastoma (GBM) accounts for half of all central nervous system tumors. Once the tumor is removed, many GBM cells remain present near the surgical cavity and infiltrate the brain up to a distance of 20 to 30 mm, resulting in recurrence a few months later. GBM remains incurable due to the limited efficiency of current treatments, a result of the blood-brain barrier and sensitivity of healthy brain tissues to chemotherapy and radiation. A new therapeutic paradigm under development to treat GBM is to attract and accumulate GBM cells in a cancer cell trap inserted in the surgical cavity after tumor resection. In this work, porous gels were prepared using porous polylactide molds obtained from melt-processed co-continuous polymer blends of polystyrene and polylactide, with an average pore size ranging from 5 µm to over 500 µm. In order to efficiently accumulate and retain glioblastoma brain cancer cells within a macroporous sodium alginate-based hydrogel trap, the pores must have an average size superior to 100 µm, with the best results obtained at 225 µm. In that case, the accumulation and retention of the F98 glioblastoma cells were more homogeneous, especially when functionalized with RGD adhesion peptides. At an alginate concentration of 1% w/v, the compression modulus reaches 15 kPa, close to the average value of 1-2 kPa reported for brain tissues, while adhesion and retention were also superior compared to 2% w/v gels. Overall, 1% w/v gels with 225 µm pores and functionalized with the RGD peptide display the best performances. .

Urethane functions can reduce metal salts under hydrothermal conditions: synthesis of noble metal nanoparticles on flexible sponges applied in semi-automated organic reduction.

We report an additive-free one-pot hydrothermal synthesis of Au, Ag, Pd, and alloy AuPd nanoparticles (NPs) anchored on commercial polyurethane (PU) foams. While unable to reduce the precursor metal salts at room temperature, PU is able to serve as a reducing agent under hydrothermal conditions. The resulting NP@PU sponge materials perform comparably to reported state-of-the-art reduction catalysts, and are additionally very well suited for use in semi-automated synthesis: the NP anchoring is strong enough and the support flexible enough to be used as a 'catalytic sponge' that can be manipulated with a robotic arm, i.e., be repeatedly dipped into and drawn out of solutions, wrung out, and re-soaked.

Affinity-controlled capture and release of engineered monoclonal antibodies by macroporous dextran hydrogels using coiled-coil interactions.

Long-term delivery is a successful strategy used to reduce the adverse effects of monoclonal antibody (mAb)-based treatments. Macroporous hydrogels and affinity-based strategies have shown promising results in sustained and localized delivery of the mAbs. Among the potential tools for affinity-based delivery systems, the de novo designed Ecoil and Kcoil peptides are engineered to form a high-affinity, heterodimeric coiled-coil complex under physiological conditions. In this study, we created a set of trastuzumab molecules tagged with various Ecoil peptides and evaluated their manufacturability and characteristics. Our data show that addition of an Ecoil tag at the C-termini of the antibody chains (light chains, heavy chains, or both) does not hinder the production of chimeric trastuzumab in CHO cells or affect antibody binding to its antigen. We also evaluated the influence of the number, length, and position of the Ecoil tags on the capture and release of Ecoil-tagged trastuzumab from macroporous dextran hydrogels functionalized with Kcoil peptide (the Ecoil peptide-binding partner). Notably, our data show that antibodies are released from the macroporous hydrogels in a biphasic manner; the first phase corresponding to the rapid release of residual, unbound trastuzumab from the macropores, followed by the affinity-controlled, slow-rate release of antibodies from the Kcoil-functionalized macropore surface.

Development and Characterization of Functional Polylactic Acid/Chitosan Porous Scaffolds for Bone Tissue Engineering.

In this study, we developed and characterized various open-cell composite scaffolds for bone regeneration. These scaffolds were made from Polylactic acid (PLA) as the scaffold matrix biopolymeric phase, and chitosan (CS) and chitosan-grafted-PLA (CS-g-PLA) copolymer as the dispersed biopolymeric phase. As a first step, successful grafting of PLA onto CS backbone was executed and confirmed by both FTIR and XPS. Mechanical characterization confirmed that adding CS or CS-g-PLA to the intrinsically rigid PLA made their corresponding PLA/CS and PLA/CS-g-PLA composite scaffolds more flexible under compression. This flexibility was higher for the latter due to the improved compatibility between PLA and CS-g-PLA copolymer. The hydrolytic stability of both PLA/CS and PLA/CS-g-PLA composite scaffolds inside phosphate-buffered saline (PBS) solution, as well as MG-63 osteoblast cell adhesion and proliferation inside both scaffolds, were characterized. The corresponding results revealed that PLA/CS composite scaffolds showed hydrolytic degradation due to the cationic properties of CS. However, modified PLA/CS-g-PLA scaffolds were hydrolytically stable due to the improved interfacial adhesion between the PLA matrix and CS-g-PLA copolymer. Finally, biological characterization was done for both PLA/CS and PLA/CS-g-PLA composite scaffolds. Contrarily to what was observed for uncompatibilized PLA/CS scaffolds, compatibilized PLA/CS-g-PLA scaffolds showed a high MG-63 osteoblast cell proliferation after three and five days of cell culture. Moreover, it was observed that cell proliferation increased with CS-g-PLA content. This suggests that the PLA/CS-g-PLA composite scaffolds could be a potential solution for bone regeneration.

Synthesis of ultrasmall metal nanoparticles and continuous shells at the liquid/liquid interface in Ouzo emulsions.

Herein, we report a novel method to synthesize metal nanoparticle-shells (NP-shells) and continuous shells at the liquid/liquid interface, via an interfacial reaction in an Ouzo emulsion. Ouzo emulsions spontaneously form submicronic droplets with a narrow size distribution, without any energy-intensive process. The Ouzo system in this work comprises water, tetrahydrofuran (THF) and butylated hydroxytoluene (BHT), and forms BHT-rich droplets (∼100 nm). The addition of a reducing agent (NaBH4) in the aqueous phase, and of a metal precursor (AuPPh3Cl and/or Pd(PPh3)2Cl2) in the BHT-rich droplets, results in the formation of Au nanoparticles (AuNPs), continuous Pd shells, or bimetallic shells, at the interface of the droplets. Control over the NP-shell size was achieved by the addition of a water-soluble polymer during the synthesis, which in turn leads to smaller NP-shells.

Macroporous dextran hydrogels for controlled growth factor capture and delivery using coiled-coil interactions.

Macroporous hydrogels possess a vast potential for various applications in the biomedical field. However, due to their large pore size allowing for unrestricted diffusion in the macropore network, macroporous hydrogels alone are not able to efficiently capture and release biomolecules in a controlled manner. There is thus a need for biofunctionalized, affinity-based gels that can efficiently load and release biomolecules in a sustained and controlled manner. For this purpose, we report here the use of a E/K coiled-coil affinity pair for the controlled capture and delivery of growth factors from highly interconnected, macroporous dextran hydrogels. By conjugating the Kcoil peptide to the dextran backbone, we achieved controlled loading and release of Ecoil-tagged Epidermal and Vascular Endothelial Growth Factors. To finely tune the behavior of the gels, we propose four control parameters: (i) macropore size, (ii) Kcoil grafting density, (iii) Ecoil valency and (iv) E/K affinity. We demonstrate that Kcoil grafting can produce a 20-fold increase in passive growth factor capture by macroporous dextran gels. Furthermore, we demonstrate that our gels can release as little as 20% of the loaded growth factors over one week, while retaining bioactivity. Altogether, we propose a versatile, highly tunable platform for the controlled delivery of growth factors in biomedical applications. STATEMENT OF SIGNIFICANCE: This work presents a highly tunable platform for growth factor capture and sustained delivery using affinity peptides in macroporous, fully interconnected dextran hydrogels. It addresses several ongoing challenges by presenting: (i) a versatile platform for the delivery of a wide range of stable, bioactive molecules, (ii) a passive, affinity-based loading of growth factors in the platform, paving the way for in situ (re)loading of the device and (iii) four different control parameters to finely tune growth factor capture and release. Altogether, our macroporous dextran hydrogels have a vast potential for applications in controlled delivery, tissue engineering and regenerative medicine.

Tailoring the Hydroxyl Density of Glass Surface for Anionic Ring-Opening Polymerization of Polyamide 6 to Manufacture Thermoplastic Composites.

Reactive thermoplastics matrices offer ease of processing using well-known molding techniques (such as Resin Transfer Molding) due to their initially low viscosity. For Polyamide 6 (PA6)/glass composites, the hydroxyl groups on the glass surface slow down the anionic ring-opening polymerization (AROP) reaction, and can ultimately inhibit it. This work aims to thoroughly control the hydroxyl groups and the surface chemistry of glass particulates to facilitate in situ AROP-an aspect that has been barely explored until now. A model system composed of a PA6 matrix synthesized by AROP is reinforced with calcinated and silanized glass microparticles. We systematically quantify, by TGA and FTIR, the complete particle surface modification sequence, from the dehydration, dehydroxylation and rehydroxylation processes, to the silanization step. Finally, the impact of the particle surface chemistry on the polymerization and crystallization of the PA6/glass composites was quantified by DSC. The results confirm that a careful balance is required between the dehydroxylation process, the simultaneous rehydroxylation and silane grafting, and the residual hydroxyl groups, in order to maintain fast polymerization and crystallization kinetics and to prevent reaction inhibition. Specifically, a hydroxyl concentration above 0.2 mmol OH·g-1 leads to a slowdown of the PA6 polymerization reaction. This reaction can be completely inhibited when the hydroxyl concentration reaches 0.77 mmol OH·g-1 as in the case of fully rehydroxylated particles or pristine raw particles. Furthermore, both the rehydroxylation and silanization processes can be realized simultaneously without any negative impact on the polymerization. This can be achieved with a silanization time of 2 h under the treatment conditions of the study. In this case, the silane agent gradually replaces the regenerated hydroxyls. This work provides a roadmap for the preparation of reinforced reactive thermoplastic materials.

Effect of Chitosan on Alginate-Based Macroporous Hydrogels for the Capture of Glioblastoma Cancer Cells.

Glioblastoma multiforme is a type of brain cancer associated with a very low survival rate since a large number of cancer cells remain infiltrated in the brain despite the treatments currently available. This work presents a macroporous hydrogel trap, destined to be implanted in the surgical cavity following tumor resection and designed to attract and retain cancer cells, in order to eliminate them afterward with a lethal dose of stereotactic radiotherapy. The biocompatible hydrogel formulation comprises sodium alginate (SA) and chitosan (CHI) bearing complementary electrostatic charges and stabilizing the gels in saline and cell culture media, as compared to pristine SA gels. The highly controlled and interconnected porosity, characterized by X-ray microCT, yields mechanical properties comparable to those of brain tissues and allows F98 glioblastoma cells to penetrate the gels within the entire volume, as confirmed by fluorescence microscopy. The addition of a grafted -RGD peptide on SA, combined with CHI, significantly enhances the adhesion and retention of F98 cells within the gels. Overall, the best compromise between low proliferation and a high level of accumulation and retention of F98 cells was obtained with the hydrogel formulated with 1% SA and 0.2% CHI, without the -RGD adhesion peptide.

Drug Delivery Systems in the Development of Novel Strategies for Glioblastoma Treatment.

Glioblastoma multiforme (GBM) is a grade IV glioma considered the most fatal cancer of the central nervous system (CNS), with less than a 5% survival rate after five years. The tumor heterogeneity, the high infiltrative behavior of its cells, and the blood-brain barrier (BBB) that limits the access of therapeutic drugs to the brain are the main reasons hampering the current standard treatment efficiency. Following the tumor resection, the infiltrative remaining GBM cells, which are resistant to chemotherapy and radiotherapy, can further invade the surrounding brain parenchyma. Consequently, the development of new strategies to treat parenchyma-infiltrating GBM cells, such as vaccines, nanotherapies, and tumor cells traps including drug delivery systems, is required. For example, the chemoattractant CXCL12, by binding to its CXCR4 receptor, activates signaling pathways that play a critical role in tumor progression and invasion, making it an interesting therapeutic target to properly control the direction of GBM cell migration for treatment proposes. Moreover, the interstitial fluid flow (IFF) is also implicated in increasing the GBM cell migration through the activation of the CXCL12-CXCR4 signaling pathway. However, due to its complex and variable nature, the influence of the IFF on the efficiency of drug delivery systems is not well understood yet. Therefore, this review discusses novel drug delivery strategies to overcome the GBM treatment limitations, focusing on chemokines such as CXCL12 as an innovative approach to reverse the migration of infiltrated GBM. Furthermore, recent developments regarding in vitro 3D culture systems aiming to mimic the dynamic peritumoral environment for the optimization of new drug delivery technologies are highlighted.

Understanding the Effect of Conformational Rigidity on Rheological Behavior and Formation of Polysaccharide-Based Hybrid Hydrogels.

The importance of conformational rigidity on macroscopic rheological properties was revealed using two model polysaccharides, namely, xanthan gum and hyaluronic acid. Xanthan gum has a rigid tertiary conformation due to its ordered double-helical structure, and the interactions between the tertiary structures result in the formation of a network/quaternary structure. In comparison, hyaluronic acid possesses a relatively flexible tertiary conformation due to its secondary random coil structure. Xanthan gum exhibits a much stronger shear thinning and more solidlike behavior compared to hyaluronic acid, owing to its network/quaternary structure. The rigid tertiary structure and the presence of a network/quaternary structure also endow xanthan gum with better resistance against environmental changes (e.g., salt and/or urea addition, temperature change) compared to hyaluronic acid. The network/quaternary structure allows xanthan gum to form gels with chitosan via electrostatic interactions when using the vapor-induced gelation technique, which is not possible for hyaluronic acid due to its flexible tertiary conformation under similar conditions.

The Polymeric Matrix Composition of Vibrio cholerae Biofilms Modulate Resistance to Silver Nanoparticles Prepared by Hydrothermal Synthesis.

Biofilms represent the dominant microbial lifestyle in nature. These complex microbial communities in which bacteria are embedded in a self-produced protective polymeric extracellular matrix, display an enhanced resistance to antimicrobials and thus represent a major health challenge. Although nanoparticles have proven to be effective against bacteria, the interactions between nanoparticles and the polymeric biofilm matrix are still unclear. In this work, silver nanoparticles (AgNPs) were used on mature biofilms formed by the pathogen Vibrio cholerae, and their effects on the biofilm microstructure were evaluated. Bacteria cells within mature biofilms showed an increased tolerance to AgNPs, with their elimination requiring a concentration nine times higher than planktonic cells. Mutant strains not able to form a pellicle biofilm were four times more susceptible to AgNPs than the wild-type strain forming a strong biofilm. Moreover, electron microscopy analysis revealed that AgNPs interacted with the extracellular matrix components and disrupted its microstructure. Finally, two major proteins, Bap1 and RbmA, appeared to mediate the biofilm bacterial resistance to AgNPs. This work highlights the role of the polymeric biofilm matrix composition in resistance to AgNPs. It underlines how crucial it is to understand and characterize the interactions between nanoparticles and the biofilm matrix, in order to design appropriate metallic nanoparticles efficient against bacterial biofilms.

An alginate-based macroporous hydrogel matrix to trap cancer cells.

To overcome the radioresistance of glioblastoma (GBM) cells infiltrated in the brain, we propose to attract these cancer cells into a trap to which a lethal radiation dose can be delivered safely. Herein, we have prepared and characterized a sodium alginate-based macroporous hydrogel as a potential cancer cell trap. Microcomputed X-ray tomography shows that the hydrogel matrices comprise interconnected pores with an average diameter of 300 µm. The F98 GBM cells migrated in the pores and mainly accumulated in the center of the matrix. Depending on the number of cancer cells added, the grafting of RGD cell-adhesion peptides to the alginate resulted in a 4 to 10 times increase in the number of F98 cells (which overexpress the associated αvß3 and αvß5 binding integrins) retained in the matrix. Finally, a radiation dose of 25 Gy eliminated all F98 cells trapped in the matrix, without significantly altering the matrix mechanical properties.

Erratum: Gascon S.; et al. Characterization and Mathematical Modeling of Alginate/Chitosan-Based Nanoparticles Releasing the Chemokine CXCL12 to Attract Glioblastoma Cells. Pharmaceutics 2020, 12, 356.

The authors wish to make the following correction to this paper [...].

Characterization and Mathematical Modeling of Alginate/Chitosan-Based Nanoparticles Releasing the Chemokine CXCL12 to Attract Glioblastoma Cells.

Chitosan (Chit) currently used to prepare nanoparticles (NPs) for brain application can be complexed with negatively charged polymers such as alginate (Alg) to better entrap positively charged molecules such as CXCL12. A sustained CXCL12 gradient created by a delivery system can be used, as a therapeutic approach, to control the migration of cancerous cells infiltrated in peri-tumoral tissues similar to those of glioblastoma multiforme (GBM). For this purpose, we prepared Alg/Chit NPs entrapping CXCL12 and characterized them. We demonstrated that Alg/Chit NPs, with an average size of ~250 nm, entrapped CXCL12 with ~98% efficiency for initial mass loadings varying from 0.372 to 1.490 µg/mg NPs. The release kinetic profiles of CXCL12 were dependent on the initial mass loading, and the released chemokine from NPs after seven days reached 12.6%, 32.3%, and 59.9% of cumulative release for initial contents of 0.372, 0.744, and 1.490 µg CXCL12/mg NPs, respectively. Mathematical modeling of released kinetics showed a predominant diffusive process with strong interactions between Alg and CXCL12. The CXCL12-NPs were not toxic and did not promote F98 GBM cell proliferation, while the released CXCL12 kept its chemotaxis effect. Thus, we developed an efficient and tunable CXCL12 delivery system as a promising therapeutic strategy that aims to be injected into a hydrogel used to fill the cavity after surgical tumor resection. This system will be used to attract infiltrated GBM cells prior to their elimination by conventional treatment without affecting a large zone of healthy brain tissue.

Mechanical and microstructural insights of Vibrio cholerae and Escherichia coli dual-species biofilm at the air-liquid interface.

Biofilm is the dominant microbial form found in nature, in which bacterial species are embedded in a self-produced extracellular matrix (ECM). These complex microbial communities are responsible for several infections when they involve multispecies pathogenic bacteria. In previous studies, interfacial rheology proved to be a unique quantitative technique to follow in real-time the biofilm formation at the air-liquid interface. In this work, we studied a model system composed of two bacteria pathogenic capable of forming a pellicle biofilm, V. cholerae and E. coli. We used an integrated approach by combining a real-time quantitative analysis of the biofilm rheological properties, with the investigation of major matrix components and the pellicle microstructure. The results highlight the competition for the interface between the two species, driven by the biofilm formation growth rate. In the dual-species biofilm, the viscoelastic properties were dominated by V. cholera, which formed a mature biofilm 18 h faster than E. coli. The microstructure of the dual-species biofilm revealed a similar morphology to V. cholerae alone when both bacteria were initially added at the same amount. The analysis of some major ECM components showed that E. coli was not able to produce curli in the presence of V. cholerae, unless enough time was given for E. coli to colonize the air-liquid interface first. E. coli secreted phosphoethanolamine (pEtN) cellulose in the dual-species biofilm, but did not form a filamentous structure. Our pathogenic model system demonstrated the importance of the biofilm growth rate for multispecies biofilm composition at the air-liquid interface.

Controlling the distribution of nanoparticles in hydrogels via interfacial synthesis.

In this article, a dual-solvent method is presented which allows for precise control over the distribution of nanoparticles (NPs) in hydrogels. The technique is based on the interfacial reaction between a reducing agent (herein THPC) initially solubilized in the hydrogel phase, and an organometallic precursor (herein Au(PPh3)Cl) solubilized in the surrounding organic liquid phase. When the organic phase is completely immiscible with water, the interfacial reaction yields a fragile monolayer film of NPs at the hydrogel surface. Then, the addition of a co-solvent (miscible with both aqueous and organic phases) allows precise tuning over the distribution of NPs, from a fine and well-anchored layer at the interface, to the whole gel volume. As a result, it is possible to independently control the size and concentration of NPs, and their distribution. The impact of such control is demonstrated with the reduction of p-nitrophenol to p-aminophenol catalyzed by gold nanoparticles (AuNPs). When AuNPs are mostly localized at the gel surface, the apparent reaction rate is more than 10× superior compared to AuNPs distributed in the whole gel - at comparable particle content and size. This approach is straightforward, decisive and compatible with broad arrays of NPs and hydrogel chemistries, and solvent combinations.

One-step processing of highly viscous multiple Pickering emulsions.

HYPOTHESIS: Solid-stabilized Pickering emulsions have attracted a lot of attention recently due to their surfactant-free character, and exceptional stability. At the moment, how the viscosities of the liquid phases impact the processing of Pickering emulsions remain to be clearly understood - it is however an important parameter to consider when developing chemical engineering processes employing these multiphase liquids. Our first assumption was that the amount of emulsified dispersed phase would drastically decrease as viscosity increases. EXPERIMENTS AND FINDINGS: In this work, we demonstrate that double water-in-oil-in-water (W/O/W) Pickering emulsions are obtained in a single processing step when using very high viscosity silicone oils (≥10,000 cSt) and a single type of sub-µm silica particles modified with two grafted silanes and sodium alginate. The formation of water sub-inclusions proceeds via a phase-inversion mechanism. These sub-inclusions are subsequently stabilized and retained in the oil phase due to its viscosity, limiting sub-inclusions mobility, and the presence of adsorbed particles forming dense layers at oil-water interfaces, acting as barriers. The process we present is simple, requires a minimum number of components, and allows the preparation of multiple emulsions which could then be used to efficiently protect and/or transport a variety of sensitive encapsulated compounds.

Microbiological and real-time mechanical analysis of Bacillus licheniformis and Pseudomonas fluorescens dual-species biofilm.

In natural habitats, bacterial species often coexist in biofilms. They interact in synergetic or antagonistic ways and their interactions can influence the biofilm development and properties. Still, very little is known about how the coexistence of multiple organisms impact the multispecies biofilm properties. In this study, we examined the behaviour of a dual-species biofilm at the air-liquid interface composed by two environmental bacteria: Bacillus licheniformis and a phenazine mutant of Pseudomonas fluorescens. Study of the planktonic and biofilm growths for each species revealed that P. fluorescens grew faster than B. licheniformis and no bactericidal effect from P. fluorescens was detected, suggesting that the growth kinetics could be the main factor in the dual-species biofilm composition. To validate this hypothesis, the single- and dual-species biofilm were characterized by biomass quantification, microscopy and rheology. Bacterial counts and microscale architecture analysis showed that both bacterial populations coexist in the mature pellicle, with a dominance of P. fluorescens. Real-time measurement of the dual-species biofilms' viscoelastic (i.e. mechanical) properties using interfacial rheology confirmed that P. fluorescens was the main contributor of the biofilm properties. Evaluation of the dual-species pellicle viscoelasticity at longer time revealed that the biofilm, after reaching a first equilibrium, created a stronger and more cohesive network. Interfacial rheology proves to be a unique quantitative technique, which combined with microscale imaging, contributes to the understanding of the time-dependent properties within a polymicrobial community at various stages of biofilm development. This work demonstrates the importance of growth kinetics in the bacteria competition for the interface in a model dual-species biofilm.

Tailored Macroporous Hydrogels with Nanoparticles Display Enhanced and Tunable Catalytic Activity.

This work demonstrates that a model system of poly( N-isopropylacrylamide) (PNIPAam) macroporous hydrogels, with tailored microstructures and comprising gold (Au) or silver (Ag) nanoparticles, display enhanced and tunable catalytic activity. These nanocomposites are prepared using polymer templates obtained from melt-processed cocontinuous polymer blends. The reaction rate, controlled by both hydrogel porosity and the PNIPAam lower critical solution temperature, increases by more than an order of magnitude as compared to nonporous gels, and is comparable to micro- or nanocarrier-based systems, with easier catalyst recovery. The fabrication process is scalable, and is compatible with broad choices of polymer blend, gel, and nanoparticle chemistries.

Sodium alginate-grafted submicrometer particles display enhanced reversible aggregation/disaggregation properties.

In this article, we demonstrate that submicrometer particles with surface-grafted sodium alginate (SA) display enhanced and reversible aggregation/disaggregation properties in aqueous solution. 300 nm silica particles were first functionalized with an aminosilane coupling agent, followed by the grafting of pH-sensitive SA, as confirmed by zeta potential, XPS and FTIR analyses. The SA-modified particles show enhanced aggregation properties at acidic pH compared to unmodified silica, with a 10 times increase in average aggregate diameter. The process is reversible, as the aggregates can be broken and dispersed again when the pH is increased back to 7.0. As a result, the sedimentation rate of SA-modified particles at pH 3.0 is both significantly faster and complete compared to the unmodified particles. This enhanced aggregation is most likely due to the formation of intermolecular hydrogen bonds between neighboring SA-modified particles. This work illustrates how surface-grafted macromolecules of natural origins can be used to tune interparticle interactions, in order to improve separation processes.