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  • 1.
    Chen, Chao
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Bactericidal Surfaces Prepared by Femtosecond Laser Patterning and Layer-by-Layer Polyelectrolyte CoatingManuskript (preprint) (Annet vitenskapelig)
    Abstract [en]

    Antimicrobial surfaces are important in medical, clinical, and industrial applications, where bacterial infection and biofouling may constitute a serious threat to human health. Conventional approaches against bacteria involve coating the surface with antibiotics, cytotoxic polymers, or metal particles. However, these types of functionalization have a limited life-time and pose concerns in terms of leaching and degradation of the coating. Thus, there is a great interest in developing long-lasting and non-leaching bactericidal surfaces. To obtain a bactericidal surface, we combine μm-scale patterning of borosilicate glass surfaces by ultrashort pulsed laser irradiation and a non-leaching layer-by-layer polyelectrolyte modification of the surface. The combination of surface structure and surface charge results in an enhanced bactericidal effect against both Gram-positive Staphylococcus aureus and Gram-negative Escherichia coli. The laser patterning and the layer-by-layer modification are environmentally friendly processes that are applicable to a wide variety of materials, which makes this method uniquely suited for fundamental studies of bacteria-surface interactions and paves the way for its applications in a variety of fields, such as in hygiene products and medical devices.

  • 2.
    Chen, Chao
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Development of Non-leaching Antibacterial Approaches on Cellulose-based Substrates and Their Mechanisms2019Doktoravhandling, med artikler (Annet vitenskapelig)
    Abstract [en]

    The layer-by-layer (LbL) technique is becoming a powerful tool that has been applied in many surface coatings and functionalizations in recent years. It has many advantages including a fast and mild process, the flexibility of choice of substrate, and the easiness to scale-up. Novel antibacterial materials can be achieved using this technique, by immobilizing selected antibacterial agents on surfaces of desired substrates. An ideal antibacterial agent, a cationic polyelectrolyte, can be LbL-deposited onto the surfaces in mono or multi layers, make the surfaces lethal to the bacteria due to their positive charge. This approach is able not only to effectively control the spreading of bacteria but also to minimize bacterial resistance as well as the environmental impact.

    Cellulose fibres modified by different cationic polyelectrolytes including PDADMAC, PAH, PVAm as either monolayer or multilayer assembled with PAA using LbL deposition have shown more than 99.99 % bacterial removal as well as the inhibition of bacterial growth. Among these modifications, two layers of PVAm assembled with one layer of PAA have shown the highest antibacterial efficiency due to the highest adsorbed amount and charge density. Secondly, PAA was replaced by a bio-based cellulose nano-fibril (CNF), as a middle layer between two layers of PVAm, which decreases the carbon-footprint and expands the possibility of using LbL technique in antibacterial applications, since the LbL technique can be used long as the alternate layers are oppositely charged. The fibres modified with this approach have shown similar and even better antibacterial properties than those of PAA.

    To develop the antibacterial approach using LbL on cellulose fibres, it is also essential to understand the antibacterial mechanism. It was found that the charge density and surface structures are two important factors affecting bacterial adhesion and the bactericidal effect. To study this, different charged cellulose model surfaces were made by coating oxidized, regenerated cellulose followed by PVAm/CNF/PVAm LbL deposition, and a better antibacterial effect was observed on the higher charged surface. By calculating the force between the bacteria and charged surface, it was suggested that a higher interaction due to the higher surface charge causes a large stress on the bacterial cell wall which leads to the disruption of the bacteria. To further improve the bactericidal effect, the flat surfaces were patterned with micro and nano structures using a femtosecond laser technique. The weakening of the bacterial cell wall caused by the charged surface makes the bacteria more vulnerable and easier to disrupt. This approach has been shown to be valid on both Gram-positive S. aureus, and Gram-negative E. coli. The effect was greater on E. coli with a weaker membrane structure and higher surface potential, which shows that the antibacterial mechanism is a physical disrupt of the bacterial cell.

  • 3.
    Chen, Chao
    et al.
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Ek, Monica
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Antibacterial evaluation of CNF/PVAm multilayer modified cellulose fiber and cellulose model surface2018Inngår i: Nordic Pulp & Paper Research Journal, ISSN 0283-2631, E-ISSN 2000-0669, Vol. 33, nr 3, s. 385-396Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Earlier studies have shown that 3-layer-modified cellulose fibers with poly(acrylic acid) (PAA) as the middle layer between two cationic polyelectrolyte polyvinylamine (PVAm) layers have strong antibacterial efficacy in terms of both bacteria adsorption and bacterial growth inhibition. In the present work, the fossil-based PAA middle layer was replaced by sustainable wood-based cellulose nano-fibrils (CNF), i. e., the fibers were modified by a 3-layer PVAm/CNF/PVAm system. Interestingly, the antibacterial efficacy of this system was greater than that of the previous PVAm/PAA/PVAm system. A higher salt concentration and lower assembly pH in the multilayer build-up resulted in better bacterial reduction. As the surface of a cellulose fiber is heterogeneous, making it difficult to characterize and visualize at high resolution, more homogeneous cellulose model surfaces were prepared by spin coating the dissolved cellulose fiber onto a silica surface to model the fiber surface. With increasing ionic strength, more aggregated and heterogeneous structures can be observed on the PVAm/CNF/PVAm modified model surfaces. The adsorbed bacteria distributed on the structured surfaces were clearly seen under fluorescence microscopy. Adsorbed amounts of bacteria on either aggregate or flat regions were quantified by scanning electron microscopy (SEM). More adsorbed bacteria were clearly seen on aggregates than on the flat regions at the surfaces. Degrees of bacteria deformation and cell damage were also seen under SEM. The surface roughness of the modified model surfaces was examined by atomic force microscopy (AFM), and a positive correlation was found between the surface roughness and the bacterial adhesion. Thus, an additional factor that controls adhesion, in addition to the surface charge, which is probably the most dominant factor affecting the bacteria adhesion, is the surface structures, such as roughness. 

  • 4.
    Chen, Chao
    et al.
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Illergård, Josefin
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Wågberg, Lars
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi, Fiberteknologi.
    Ek, Monica
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Effect of cationic polyelectrolytes in contact-active antibacterial layer-by-layer functionalization2017Inngår i: Holzforschung, ISSN 0018-3830, E-ISSN 1437-434X, Vol. 71, nr 7-8, s. 649-658Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Contact-active surfaces have been created by means of the layer-by-layer (LbL) modification technique, which is based on previous observations that cellulose fibers treated with polyelectrolyte multilayers with polyvinylamine (PVAm) are perfectly protected against bacteria. Several different cationic polyelectrolytes were applied, including PVAm, two different poly(diallyl dimethyl ammonium chloride) polymers and two different poly(allylamine hydrochloride) polymers. The polyelectrolytes were self-organized in one or three layers on cellulosic fibers in combination with polyacrylic acid by the LbL method, and their antibacterial activities were evaluated. The modified cellulose fibers showed remarkable bacterial removal activities and inhibited bacterial growth. It was shown that the interaction between bacteria and modified fibers is not merely a charge interaction because a certain degree of bacterial cell deformation was observed on the modified fiber surfaces. Charge properties of the modified fibers were determined based on polyelectrolyte titration and zeta potential measurements, and a correlation between high charge density and antibacterial efficiency was observed for the PVAm and PDADMAC samples. It was demonstrated that it is possible to achieve antibacterial effects by the surface modification of cellulosic fibers via the LbL technique with different cationic polyelectrolytes.

  • 5.
    Chen, Chao
    et al.
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Pettersson, Torbjörn
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Illergård, Josefin
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Ek, Monica
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Wågberg, Lars
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi, Fiberteknologi.
    Influence of Cellulose Charge on Bacteria Adhesion and Viability to PVAm/CNF/PVAm-Modified Cellulose Model Surfaces2019Inngår i: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    A contact-active antibacterial approach based on the physical adsorption of a cationic polyelectrolyte onto the surface of a cellulose material is today regarded as an environment-friendly way of creating antibacterial surfaces and materials. In this approach, the electrostatic charge of the treated surfaces is considered to be an important factor for the level of bacteria adsorption and deactivation/killing of the bacteria. In order to clarify the influence of surface charge density of the cellulose on bacteria adsorption as well as on their viability, bacteria were adsorbed onto cellulose model surfaces, which were modified by physically adsorbed cationic polyelectrolytes to create surfaces with different positive charge densities. The surface charge was altered by the layer-by-layer (LbL) assembly of cationic polyvinylamine (PVAm)/anionic cellulose nanofibril/PVAm onto the initially differently charged cellulose model surfaces. After exposing the LbL-treated surfaces to Escherichia coli in aqueous media, a positive correlation was found between the adsorption of bacteria as well as the ratio of nonviable/viable bacteria and the surface charge of the LbL-modified cellulose. By careful colloidal probe atomic force microscopy measurements, it was estimated, due to the difference in surface charges, that interaction forces at least 50 nN between the treated surfaces and a bacterium could be achieved for the surfaces with the highest surface charge, and it is suggested that these considerable interaction forces are sufficient to disrupt the bacterial cell wall and hence kill the bacteria.

  • 6.
    Huang, Tianxiao
    et al.
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi, Träkemi och massateknologi.
    Chen, Chao
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Li, Dongfang
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Ek, Monica
    KTH, Skolan för kemi, bioteknologi och hälsa (CBH), Fiber- och polymerteknologi.
    Hydrophobic and antibacterial textile fibres prepared by covalently attaching betulin to cellulose2019Inngår i: Cellulose (London), ISSN 0969-0239, E-ISSN 1572-882X, Vol. 26, nr 1, s. 665-677Artikkel i tidsskrift (Fagfellevurdert)
    Abstract [en]

    Betulin, a natural compound extractable from the outer bark of birch, can be used to improve the properties of cellulosic textile fibres. Herein, oxidation was performed to prepare carboxyl-functionalized cellulose, which was subsequently covalently attached by betulin through esterification. The surface-modified cellulosic textile fibres showed a substantially improved hydrophobicity, as indicated by a water contact angle of 136°. Moreover, the material showed excellent antibacterial properties, as indicated by over 99% bacterial removal and growth inhibition, in both Gram-positive and Gram-negative bacterial assays. The method of surface-modification of the cellulosic materials adapted in this study is simple and, to the best of our knowledge, has not been carried out before. The results of this study prove that betulin, a side-stream product produced by forest industry, could be used in value-added applications, such as for preparing functional materials. Additionally, this modification route can be envisaged to be applied to other cellulose sources (e.g., microfibrillated cellulose) to achieve the goal of functionalization.

  • 7.
    Ottenhall, Anna
    et al.
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Chen, Chao
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Henschen, Jonatan
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Illergård, Josefin
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Larsson, Per A.
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Wågberg, Lars
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Ek, Monica
    KTH, Skolan för kemivetenskap (CHE), Fiber- och polymerteknologi.
    Layer-by-layer modification of cellulosic materials for green antibacterial materials2017Inngår i: Abstracts of Papers of the American Chemical Society, ISSN 0065-7727, Vol. 253Artikkel i tidsskrift (Annet vitenskapelig)
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