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.

Filtration is a common way to obtain pure drinking water by removing particles and microorganisms based on size exclusion. Cellulose-based filters are affordable and biobased option for the removal of particles but bacteria are usually too small to be removed by size exclusion alone. In this article, the surfaces of cellulose fibres in two types of commercial paper filters have been given a positive net charge to trap bacteria through electrostatic interactions without releasing any biocides. The fibres were modified with the cationic polyelectrolyte polyvinylamine polymer in single layers (1 L) or in multilayers together with the anionic polyelectrolyte polyacrylic acid (3 L or 5 L) using a water-based process at room temperature. Filtration tests show that all filters, using both types of filter papers and a number of layers, can physically remove more than 99.9% of E. coli from water and that the 3 L modified filters can remove more than 97% of cultivatable bacteria from natural water samples. The bacterial reduction increased with increasing number of filter sheets used for the filtration and the majority of the bacteria were trapped in the top sheets of the filter. The results show the potential for creating water purification filters from bio-based everyday consumable products with a simple modification process. The filters could be used in the future for point-of-use water purification that may be able to save lives without releasing bactericides.

Cellulose nanofibril (CNF) materials have been widely studied in recent years and are suggested for a wide range of applications, e.g., medical and hygiene products. One property not very well studied is the interaction between bacteria and these materials and how this can be controlled. The current work studies how bacteria adhere to different CNF materials modified with polyelectrolyte multilayers. The tested materials were TEMPO-oxidized to have different surface charges, periodate-oxidized to vary the water interaction and hot-pressed to alter the surface structure. Then, multilayers were constructed using polyvinylamine (PVAm) and polyacrylic acid. Both the material surface charge and water interaction affect the amount of polymer adsorbed to the surfaces. Increasing the surface charge decreases the adsorption after the first PVAm layer, possibly due to conformational changes. Periodate-oxidized and crosslinked films have low initial polymer adsorptions; the decreased swelling prevents polymer diffusion into the CNF micropore structure. Microscopic analysis after incubating the samples with bacterial suspensions show that only the materials with the lowest surface charge enable bacteria to adhere to the surface because, when adsorbing up to 5 layers PVAm/PAA, the increased anionic surface charge appears to decrease the net surface charge. Both the amounts of PVAm and PAA influence the net surface charge and thus the bacterial adhesion. The structure generated by the hot-pressing of the films also strongly increases the number of bacteria adhering to the surfaces. These results indicate that the bacterial adhesion to CNF materials can be tailored using polyelectrolyte multilayers on different CNF substrates.

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.

 Portable purifi cation systems are easy ways to obtain clean drinking water when there is no large-scale water treatment available. In this study, the potential to purify water using bacteria adsorbing cellulosic fi bers, functionalized with polyelectrolytes according to the layer-by-layer method, is investigated. The adsorbed polyelectrolytes create a positive charge on the fi ber surface that physically attracts and bonds with bacteria. Three types of cellulosic materials have been modifi ed and tested for the bacterial removal capacity in water. The time, material-water ratio and bacterial concentration dependence, as well as the bacterial removal capacity in water from natural sources, have been evaluated. Freely dispersed bacteria adsorbing cellulosic fi bers can remove greater than 99.9% of Escherichia coli  from nonturbid water, with the most notable reduction occurring within the fi rst hour. A fi ltering approach using modifi ed cellulosic fi bers is desirable for purifi cation of natural water. An initial fi ltration test showed that polyelectrolyte multilayer modifi ed cellulosic fi bers can remove greater than 99% of bacteria from natural water. The bacteria adsorbing cellulosic fi bers do not leach any biocides, and it is an environmentally sustainable and cheap option for disposable water purification devices.

The use of cellulose aerogels as antibacterial materials has been investigated by applying a contact-active layer-by-layer modification to the aerogel surface. Studying the adsorption of multilayers of polyvinylamine (PVAm) and polyacrylic acid to aerogels comprising crosslinked cellulose nanofibrils and monitoring the subsequent bacterial adhesion revealed that up to 26 mg PVAm g aerogel⁻¹ was adsorbed without noticeably affecting the aerogel structure. The antibacterial effect was tested by measuring the reduction of viable bacteria in solution when the aerogels were present. The results show that >99.9% of the bacteria adhered to the surface of the aerogels. Microscopy further showed adherence of bacteria to the surfaces of the modified aerogels. These results indicate that it is possible to create materials with three-dimensional cellulose structures that adsorb bacteria with very high efficiency utilizing the high specific surface area of the aerogels in combination with their open structure.