IN-SITU PATTERNING OF FIBRE ARTICLES

Description

The present invention relates to methods for preparing a crease patterned fibre article, a crease patterned fibre article obtainable by said method as well as the use of a crease patterned fibre article as a packaging, design article, fabrics, bio-tissue implant, organ substitute, organ regeneration (patch), organ model, tissue substitute, tissue model, tissue scaffolds, cell growth support, cell maturing support or bone reinforcement.

Origami paper folding is a very well-known technique, which is used to shape robust and reliable 3D-shaped articles such as animals and flowers from a flat sheet of paper. By this technique, only a very small part of the paper sheet is deformed when it is creased, but the existence of such crease readily changes its deformation modes in that the formed article is robust and reliable against mechanical action to some extent.

For example, reference can be made to the references of Ahmed, A. R., Gauntlett, O. C., and Camci-Unal, G.; “Origami-Inspired Approaches for Biomedical Applications”. ACS Omega 2021, 6, 46-54. Reid, A., Lechenault, F., Rica, S., and Adda-Bedia, M.; “Geometry and design of origami bellows with tunable response”; Physical Review E, 2017, 95(1), 013002. Kuribayashi-Shigetomi, Kaori, Hiroaki Onoe, and Shoji Takeuchi; “Cell origami: self-folding of three-dimensional cell-laden microstructures driven by cell traction force”; PLOS ONE, December 2012, Vol. 7, Issue 12. Py, C., et al. “Capillary origami: spontaneous wrapping of a droplet with an elastic sheet.” Physical review letters, 2017, 98(15), 156103

However, preparing an article by the origami technique, i.e. by folding a ready-to-use paper or paperboard, is not feasible for production at industrial scale.

Therefore, there is an ongoing need for a method for preparing a crease patterned fibre article such as a crease patterned paper or paperboard.

Accordingly, it is an object of the present invention to provide a method for preparing a crease patterned fibre article. Furthermore, it is desirable that the method is specifically suitable for preparing a crease patterned paper or paperboard. Furthermore, it is desirable that the method for preparing a crease patterned fibre article is feasible for producing such fibre articles at industrial scale. Furthermore, it is desirable that the obtained crease patterned fibre article can be used as a packaging, design article, fabrics, bio-tissue implant, organ substitute, organ regeneration (patch), organ model, tissue substitute, tissue model, tissue scaffolds, cell growth support, cell maturing support or bone reinforcement.

The foregoing and other objects are solved by the subject-matter as defined in the independent claims. Advantageous embodiments of the present invention are defined in the corresponding subclaims.

According to one aspect of the present invention, a method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, is provided. The method comprising the steps of

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres,
  • c) depositing the aqueous suspension comprising fibres onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article.

According to another aspect, a method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, is provided. The method comprising the steps of

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres,
  • c1) depositing the aqueous suspension comprising fibres onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using the crease patterning device to form a patterned fibre web, and
    • d) drying the patterned fibre web to obtain the crease patterned fibre article.

According to one embodiment, the crease patterning device is made from a material selected from the group comprising alloy and non-alloy steel, cast steel, cast iron, aluminium, ceramics, sintered metal, brass, titanium, copper and polymer materials.

According to another embodiment, the crease patterning device is a mesh, preferably a wire mesh, most preferably a wire mesh containing a crease pattern.

According to another embodiment, the wire mesh comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm, and/or an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm; and/or an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm.

According to one embodiment, the crease pattern of the crease patterning device is created by engraving, laid wires, chain wires, soldering, embossing, 3D printing or melt moulding, preferably embossing e.g. of a brass mesh.

According to another embodiment, the aqueous suspension comprises the fibres in an amount ranging from 0.5 to 30 wt.-%, based on the total weight of the aqueous suspension, preferably from 0.5 to 25 wt.-%, more preferably from 0.5 to 20 wt.-% and most preferably from 0.5 to 15 wt.-%.

According to yet another embodiment, the fibres in the aqueous suspension are biocompatible and/or the fibres in the aqueous suspension comprise cellulose, preferably the fibres comprising cellulose are contained in pulps selected from the group comprising eucalyptus pulp, spruce pulp, pine pulp, beech pulp, hemp pulp, cotton pulp, wheat pulp, oat pulp, rye pulp, barley pulp, rice pulp, bamboo pulp, bagasse pulp, miscanthus pulp, sisal pulp, jute pulp, acacia pulp, birch pulp and mixtures thereof.

According to one embodiment, the fibres in the aqueous suspension have an average diameter ranging from 1 to 35 μm, preferably from 2 to 30 μm and most preferably from 3 to 20 μm, and/or an average length ranging from 0.7 to 250 mm, preferably from 0.8 to 230 mm and most preferably from 0.9 to 200 mm.

According to another embodiment, the depositing in step c) or step c1) is carried out by jetting, casting, spray coating, curtain coating, slide bed coating, film pressing, metered film pressing, blade coating, brush coating or paper press forming.

According to yet another embodiment, drying step d) is carried out under vacuum and/or a temperature ranging from 80 to 200° C., preferably from 85 to 180° C. and most preferably from 90 to 150° C.

According to one embodiment, the process comprises a further step e) of separating the crease patterned fibre article from the crease patterning device and/or wire mesh.

According to another embodiment, the process comprises a further step f) of folding the crease patterned fibre article into a 3D shape.

According to yet another embodiment, the process comprises a further step g) of applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article.

According to one embodiment, the cells and/or enzymes and/or pharmaceuticals are provided in a carrier material, preferably the carrier material is selected from the group comprising gelatin, methylcellulose, alginate, agarose, fibrin, hyaluronic acid, K-carrageenan, poly(ethylene glycol) (PEG), polycaprolactone (PCL), matrigel, gelatin methacrylate, poloxamer, nanocellulose, peptide, silk fibroin and mixtures thereof.

According to another aspect of the present invention, a crease patterned fibre article, preferably a crease patterned paper or paperboard, obtainable by a method as described herein, is provided.

According to one embodiment, the article is a packaging, design article, fabrics, bio-tissue implant, organ substitute, organ regeneration (patch), organ model, tissue substitute, tissue model, tissue scaffolds, cell growth support, cell maturing support or bone reinforcement.

According to another aspect of the present invention, the use of a crease patterned fibre article as a packaging, design article, fabrics, bio-tissue implant, organ substitute, organ regeneration (patch), organ model, tissue substitute, tissue model, tissue scaffolds, cell growth support, cell maturing support or bone reinforcement is provided.

It should be understood that for the purpose of the present invention, the following terms have the following meaning:

The term “biocompatible” in the meaning of the present invention refers to a material that is in accordance with EN ISO 10993-1:2021-05. Thus, the term “biocompatible” refers to the ability of a medical device (3.14) or material (3.12) to perform with an appropriate host response in a specific application. In general, biocompatible materials (3.12) are defined as being a synthetic or natural polymer, metal or alloy, ceramic, or composite, including tissue rendered nonviable, used as a medical device (3.14) or any part thereof.

Where an indefinite or definite article is used when referring to a singular noun, e.g., “a”, “an” or “the”, this includes a plural of that noun unless anything else is specifically stated.

Where the term “comprising” is used in the present description and claims, it does not exclude other elements. For the purposes of the present invention, the term “consisting of” is considered to be a preferred embodiment of the term “comprising”. If hereinafter a group is defined to comprise at least a certain number of embodiments, this is also to be understood to disclose a group, which preferably consists only of these embodiments.

Terms like “obtainable” or “definable” and “obtained” or “defined” are used interchangeably. This, for example, means that, unless the context clearly dictates otherwise, the term “obtained” does not mean to indicate that, for example, an embodiment must be obtained by, for example, the sequence of steps following the term “obtained” though such a limited understanding is always included by the terms “obtained” or “defined” as a preferred embodiment.

Whenever the terms “including” or “having” are used, these terms are meant to be equivalent to “comprising” as defined hereinabove.

The method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, of the present invention comprises the steps of

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article.

Alternatively, the method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, of the present invention comprises the steps of

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article.

In the following, preferred embodiments of the inventive methods will be set out in more detail. It is to be understood that these embodiments and details also apply to the inventive products obtainable by said methods and their uses described herein.

The invention refers to a method for preparing a crease patterned fibre article. The crease patterned fibre article is preferably a crease patterned paper or paperboard.

According to step a) of the methods for preparing a crease patterned fibre article, a crease patterning device is provided.

In the meaning of the present invention, a “crease patterning device” is a device creating a crease patterning on a fibre web that is treated with such a device. Furthermore, the crease patterning device should be in a condition such that the crease pattern can be reliably created in the fibre web without deformations and failures in the crease pattern. In addition, thereto, the crease patterning device should be (chemically) stable in that it is neither reacting with the moisture nor the fibres in the fibre web that is treated with the crease patterning device (at least for the period of the method). Furthermore, the crease patterning device should be mechanically and thermally stable at temperatures of up to about 120° C.

Thus, the crease patterning device can be made of any material that is rigid and (chemically) stable. Examples of materials include but are not limited to inert metals and alloys, ceramics and polymer materials.

In one embodiment, the crease patterning device is made from a material selected from the group comprising alloy and non-alloy steel, cast steel, cast iron, aluminium, ceramics, sintered metal, brass, titanium, copper and polymer materials.

If the crease patterning device is made of a polymer material. The polymer material can be e.g. selected from biocompatible resins, thermoplastics and duroplasts. For example, the polymer material can be selected from acrylonitrile butadiene styrene (ABS), polycarbonate (PC) and polycarbonate blends with biomaterials or fossil-fuel, polyether ether ketone (PEEK), polyethylene terephthalate glycol (PETG), polylactic acid (PLA), polyamide 12 (also known as Nylon 12), (meth)acrylic-based polymers, epoxy-based polymers and polyurethane, such as thermoplastic polyurethane. Preferably, the polymer material is polycarbonate (PC). Alternatively, the polymer material is polylactic acid (PLA). Such materials are very well known in the art and the skilled person is well aware of how such polymer material is selected for the desired purpose.

In a preferred embodiment, the crease patterning device is made from a material selected from the group comprising non-alloy steel, ceramics, copper and polymer materials.

If the crease patterning device is made of a metal or alloy, the crease patterning device is preferably a mesh, preferably a wire mesh. In this embodiment, the crease patterning device is thus preferably a wire mesh containing a crease pattern.

For example, the crease patterning device in the form of a wire mesh is made of steel or copper.

In one embodiment, the wire mesh comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm.

Additionally or alternatively, the wire mesh has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm.

In one embodiment, the wire mesh has an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm.

In a preferred embodiment, the wire mesh has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm, and an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm.

For example, the wire mesh comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm, or the wire mesh has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm, and an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 25 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm. Alternatively, the wire mesh comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm, and the wire mesh has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm, and an amount of weft wires ranging from 200 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm.

In one embodiment, the wire mesh has a similar amount of warp wires/cm and weft wires/cm, i.e. the amount of warp and weft wires is similar and ranges from 20 to 90 warp and weft wires/cm, preferably from 20 to 80 warp and weft wires/cm and most preferably from 20 to 70 warp and weft wires/cm, e.g. from 40 to 65 warp and weft wires/cm.

It is appreciated that the wording “similar” amount of warp wires/cm and weft wires/cm throughout the present invention means that the amount of warp wires/cm and weft wires/cm differ by at most 10/cm, more preferably by at most 8/cm and most preferably by at most 6/cm. If the crease patterning device is made of a ceramic or polymer material such as a biocompatible resins or polycarbonate or polylactic acid, the crease patterning device is preferably a mould. In this embodiment, the crease patterning device is thus preferably a mould containing a crease pattern.

It is to be noted that the crease pattern of the crease patterning device can be achieved by any method known in the art for creating such a pattern on a device. For example, the crease pattern of the crease patterning device is created by engraving, laid wires, chain wires, soldering, embossing, 3D printing or melt moulding, preferably embossing e.g. of a brass mesh. Such methods are well known and do not need to be described in more detail herein.

The crease pattern created by the crease patterning device may be any pattern known to the skilled person that is suitable to be further folded into a 3D shape. For example, the crease pattern is selected from the Miura pattern, Miura Ori pattern, Yoshimura pattern, waterbomb pattern, Ron Resch pattern, Glide Reflection (GR, GR2) pattern, and mixtures and derivatives thereof. Preferably, the crease pattern created by the crease patterning device is the Miura pattern or Yoshimura pattern. Preferably, the crease pattern created by the crease patterning device is the Miura pattern.

It is to be noted that the crease pattern created by the crease patterning device on fibre article can be created on only a part or the whole fibre article.

According to step b) of the methods, an aqueous suspension comprising fibres is provided.

It is appreciated that the amount of fibres in the aqueous suspension may vary in a broad range. However, it is preferred that the amount of fibres in the aqueous suspension is such that the fibres can be easily deposited on the crease patterning device or wire mesh in step c). Furthermore, it is preferred that the amount of solvent in the aqueous suspension is such that the water consumption and the energy required for filtrating in step c) or step c1) is as low as possible.

In general, the aqueous suspension thus comprises the fibres, preferably the biocompatible fibres, in an amount ranging from 0.5 to 30 wt.-%, based on the total weight of the aqueous suspension. Preferably, the aqueous suspension thus comprises the fibres, preferably the biocompatible fibres, in an amount ranging from 0.5 to 25 wt.-%, more preferably from 0.5 to 20 wt.-% and most preferably from 0.5 to 15 wt.-%, based on the total weight of the aqueous suspension. For example, the aqueous suspension comprises the fibres, preferably the biocompatible fibres, in an amount ranging from 0.5 to 10 wt.-%, based on the total weight of the aqueous suspension.

The fibres in the aqueous suspension are not restricted to a specific type of fibres. In general any kind of fibre that is suitable for preparing fibre articles such as paper or paperboard can be used in the methods of the present invention. More precisely, any fibre that is suitable for the desired article and its corresponding use can be used in the aqueous suspension.

Preferably, the fibres in the aqueous suspension are biocompatible.

The term “biocompatible” fibres refers to fibres that do not exert a negative impact, i.e. they are not harmful or toxic, on (living) tissue or cell viability. Preferably, the biocompatible fibres do not exert a negative impact on the viability of (living) cells such as cardiovascular cells, e.g. endothelial cells, vascular smooth muscle cells, lymphatic endothelial cells, cardiomyocytes, and atherosclerosis cells, or skin cells, e.g. keratinocytes, melanocytes, Langerhans cells, and Merkel cells, or bone cells, e.g. osteoblasts, osteocytes, osteoclasts, and osteoprogenitor cells and/or enzymes such as transglutaminase enzyme.

Additionally or alternatively, the fibres in the aqueous suspension comprise cellulose.

In one embodiment, the fibres in the aqueous suspension are biocompatible or the fibres in the aqueous suspension comprise cellulose.

Alternatively, the fibres in the aqueous suspension are biocompatible and the fibres in the aqueous suspension comprise cellulose.

It is preferred that the fibres, preferably the biocompatible fibres, comprising cellulose are contained in pulps selected from the group comprising eucalyptus pulp, spruce pulp, pine pulp, beech pulp, hemp pulp, cotton pulp, including cotton linters, wheat pulp, oat pulp, rye pulp, barley pulp, rice pulp, bamboo pulp, bagasse pulp, miscanthus pulp, sisal pulp, jute pulp, acacia pulp, birch pulp, fir pulp, lyocell pulp and mixtures thereof. In one embodiment, the fibres, preferably the biocompatible fibres, comprising cellulose are contained in eucalyptus pulp or in cotton pulp. For example, the fibres, preferably the biocompatible fibres, comprising cellulose are contained in cotton pulp.

In one embodiment, the fibres, preferably the biocompatible fibres, comprising cellulose are contained in a mixture of pulps comprising two or more pulps selected from the group comprising eucalyptus pulp, spruce pulp, pine pulp, beech pulp, hemp pulp, cotton pulp, wheat pulp, oat pulp, rye pulp, barley pulp, rice pulp, bamboo pulp, bagasse pulp, miscanthus pulp, sisal pulp, jute pulp, acacia pulp, birch pulp, fir pulp and lyocell pulp. For example, the fibres, preferably the biocompatible fibres, comprising cellulose are contained in a mixture of pine pulp and spruce pulp, preferably a mixture comprising about 20 to 30 wt.-% pine pulp and 70 to 80 wt.-% of spruce pulp, based on the total weight of the mixture.

In view of this, the fibres, preferably the biocompatible fibres, in the aqueous suspension are selected from the group comprising eucalyptus fibres, spruce fibres, pine fibres, beech fibres, hemp fibres, cotton fibres, cotton linters, wheat fibres, oat fibres, rye fibres, barley fibres, rice fibres, bamboo fibres, bagasse fibres, miscanthus fibres, sisal fibres, jute fibres, acacia fibres, birch fibres, fir fibres, lyocell fibres, viscose fibres and mixtures thereof. In one embodiment, the fibres, preferably the biocompatible fibres, in the aqueous suspension are eucalyptus fibres or cotton fibres or cotton linters. For example, the fibres, preferably the biocompatible fibres, in the aqueous suspension are cotton fibres or cotton linters.

In one embodiment, the fibres, preferably the biocompatible fibres, in the aqueous suspension are a mixture of fibres comprising two or more fibres, preferably the biocompatible fibres, selected from the group comprising eucalyptus fibres, spruce fibres, pine fibres, beech fibres, hemp fibres, cotton fibres, cotton linters, wheat fibres, oat fibres, rye fibres, barley fibres, rice fibres, bamboo fibres, bagasse fibres, miscanthus fibres, sisal fibres, jute fibres, acacia fibres, birch fibres, fir fibres, viscose fibres and lyocell fibres. For example, the fibres, preferably the biocompatible fibres, in the aqueous suspension are a mixture of pine fibres and spruce fibres, preferably a mixture comprising about 20 to 30 wt.-% pine fibres and 70 to 80 wt.-% of spruce fibres, based on the total weight of the mixture.

It is appreciated that the fibres in the aqueous suspension preferably consist of biocompatible fibres. Thus, the biocompatible fibres are preferably free of fibres that are bio-incompatible.

It is appreciated that the fibres, preferably the biocompatible fibres, have dimensions that are typically observed for the articles to be prepared.

Thus, the fibres, preferably the biocompatible fibres, in the aqueous suspension preferably have an average diameter ranging from 1 to 35 μm, preferably from 2 to 30 μm and most preferably from 3 to 20 μm.

Additionally or alternatively, the fibres, preferably the biocompatible fibres, in the aqueous suspension preferably have an average length ranging from 0.7 to 250 mm, preferably from 0.8 to 230 mm and most preferably from 0.9 to 200 mm. In one embodiment, the fibres, preferably the biocompatible fibres, in the aqueous suspension preferably have an average length ranging from 0.8 to 250 mm, preferably from 1 to 230 mm and most preferably from 2 to 200 mm.

For example, the fibres, preferably the biocompatible fibres, in the aqueous suspension have an average diameter ranging from 1 to 35 μm, preferably from 2 to 30 μm and most preferably from 3 to 20 μm or an average length ranging from 0.7 to 250 mm, preferably from 0.8 to 230 mm and most preferably from 0.9 to 200 mm. In another embodiment, the fibres, preferably the biocompatible fibres, in the aqueous suspension have an average diameter ranging from 1 to 35 μm, preferably from 2 to 30 μm and most preferably from 3 to 20 μm and an average length ranging from 0.7 to 250 mm, preferably from 0.8 to 230 mm and most preferably from 0.9 to 200 mm.

In one embodiment, the fibres, preferably the biocompatible fibres, in the aqueous suspension have an average diameter ranging from 1 to 35 μm, preferably from 2 to 30 μm and most preferably from 3 to 20 μm or an average length ranging from 0.8 to 250 mm, preferably from 1 to 230 mm and most preferably from 2 to 200 mm. In another embodiment, the fibres, preferably the biocompatible fibres, in the aqueous suspension have an average diameter ranging from 1 to 35 μm, preferably from 2 to 30 μm and most preferably from 3 to 20 μm and an average length ranging from 0.8 to 250 mm, preferably from 1 to 230 mm and most preferably from 2 to 200 mm.

The solvent of the aqueous suspension comprises water, optionally in admixture with an organic solvent such as methanol, ethanol, n-butanol, isopropanol, n-propanol, acetone, dimethylsulphoxide, dimethylformamide, tetrahydrofurane, and mixtures thereof. Preferably, the solvent is water, methanol, ethanol and/or acetone. More preferably, the solvent comprises, most preferably consists of, water.

It is to be noted that the aqueous suspension comprising fibres, preferably biocompatible fibres, may further comprise typical additives used in the paper making process. For example, the aqueous suspension may comprise lignin as additive.

According to step c) of the method, the aqueous suspension comprising fibres, preferably biocompatible fibres, is deposited onto one surface of the crease patterning device and the aqueous suspension is filtrated to form a patterned fibre web.

The aqueous suspension comprising fibres, preferably biocompatible fibres, can be deposited onto one surface of the crease patterning device by any method known in the art. For example, the depositing in step c) is carried out by jetting, casting, spray coating, curtain coating, slide bed coating, film pressing, metered film pressing, blade coating, brush coating or paper press forming. A preferred method in step c) is jetting, preferably jetting into a paper machine's headbox.

It is to be noted that the aqueous suspension comprising fibres, preferably biocompatible fibres, is deposited onto one surface of the crease patterning device. In this regard, it is advantageous if the crease patterning device is provided in a horizontal or almost horizontal position such that the fibres, preferably the biocompatible fibres, in the aqueous suspension can be evenly distributed on the surface of the crease patterning device.

The aqueous suspension is then filtrated to form a patterned fibre web on the crease patterning device. More precisely, the patterned fibre web is primarily formed through removal of the solvent, e.g. water, from the aqueous suspension comprising fibres, preferably biocompatible fibres, via filtration. The filtration in step c) can be done without further aids, i.e. by gravity only. Alternatively, the filtration in step c) is done by applying vacuum or partial vacuum. The vacuum or partial vacuum may be advantageous in order to speed up the formation of the patterned fibre web on the surface of the crease patterning device. That is to say, the vacuum or partial vacuum is applied opposite to the surface onto which the aqueous suspension comprising fibres is deposited.

Step c) is preferably carried out at room temperature, temperatures ranging from 20 to 24° C., but it is also possible to carry out method step c) at higher temperatures such as from 25 to 50° C.

According to an alternative step c1) of the method, the aqueous suspension comprising fibres, preferably biocompatible fibres, is deposited onto a wire mesh and the aqueous suspension is filtrated to form a fibre web and in step c2), the fibre web is then patterned by using the crease patterning device to form a patterned fibre web.

The wire mesh of method step c1) can be a wire mesh containing a crease pattern or a wire mesh without a crease pattern. Preferably, the wire mesh of method step c1) is a wire mesh without a crease pattern.

The wire mesh of method step c1) is preferably made of steel or copper. However, any other material that is inert with respect to the aqueous suspension comprising fibres may be also suitable.

In one embodiment, the wire mesh of method step c1) comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm.

Additionally or alternatively, the wire mesh of method step c1) has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm.

In one embodiment, the wire mesh of method step c1) has an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm.

In a preferred embodiment, the wire mesh of method step c1) has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm, and an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm.

For example, the wire mesh of method step c1) comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm, or the wire mesh has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm, and an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 weft wires/cm. Alternatively, the wire mesh comprises wires having a diameter ranging from 20 to 500 μm, preferably from 40 to 450 μm and most preferably from 50 to 400 μm, and the wire mesh has an amount of warp wires ranging from 20 to 90 warp wires/cm, preferably from 20 to 80 warp wires/cm and most preferably from 20 to 70 warp wires/cm, e.g. from 40 to 65 warp wires/cm, and an amount of weft wires ranging from 20 to 90 weft wires/cm, preferably from 20 to 80 weft wires/cm and most preferably from 20 to 70 weft wires/cm, e.g. from 40 to 65 warp wires/cm.

In one embodiment, the wire mesh of method step c1) has a similar amount of warp wires/cm and weft wires/cm, i.e. the amount of warp and weft wires is similar and ranges from 20 to 90 warp and weft wires/cm, preferably from 20 to 80 warp and weft wires/cm and most preferably from 20 to 70 warp and weft wires/cm, e.g. from 40 to 65 warp and weft wires/cm.

The aqueous suspension comprising fibres, preferably biocompatible fibres, can be deposited onto the wire mesh by any method known in the art. For example, the depositing in step c1) is carried out by jetting, casting, spray coating, curtain coating, slide bed coating, film pressing, metered film pressing, blade coating, brush coating or paper press forming. A preferred method in step c1) is jetting, preferably jetting into a paper machine's headbox.

It is to be noted that the aqueous suspension comprising fibres, preferably biocompatible fibres, is deposited onto the wire mesh. In this regard, it is advantageous if the wire mesh is provided in a horizontal or almost horizontal position such that the fibres, preferably the biocompatible fibres, in the aqueous suspension can be evenly distributed on the wire mesh.

The aqueous suspension is then filtrated to form a fibre web on the wire mesh. The fibre web is primarily formed through removal of the solvent from the aqueous suspension comprising fibres, preferably biocompatible fibres, via filtration. The filtration in step c1) can be done without further aids, i.e. by gravity only. Alternatively, the filtration in step c1) is done by applying vacuum or partial vacuum. The vacuum or partial vacuum may be advantageous in order to speed up the formation of the fibre web onto the wire mesh. That is to say, the vacuum or partial vacuum is applied opposite to the surface onto which the aqueous suspension comprising fibres is deposited.

It is to be noted that the wire mesh of step c1) is preferably unpatterned such that the fibre web formed on the wire mesh by filtration is also preferably unpatterned.

According to method step c2), the fibre web is then patterned by using the crease patterning device to form a patterned fibre web

If the wire mesh used in method step c1) is a patterned wire mesh, it is appreciated that the wire mesh and the crease patterning device provide the positive and negative form of the pattern.

If the wire mesh used in method step c2) is an unpatterned wire mesh, it is appreciated that the wire mesh must be configured such that the pattern can be created in the fibre web via the crease patterning device. That is to say, the wire mesh must be configured such that it gives in under pressure of the crease patterning device and thus adapts to the form of said device and thus creating the pattern into the fibre web.

Steps c1) and c2) are preferably carried out at room temperature, temperatures ranging from 20 to 24° C., but it is also possible to carry out method steps c1) and c2) at higher temperatures such as from 25 to 50° C.

In view of the above, it is appreciated that the patterned fibre web formed in step c) or the fibre web formed in step c1) has a higher content of fibres, preferably biocompatible fibres, compared to the aqueous suspension comprising the fibres, preferably the biocompatible fibres, which is deposited on the crease patterning device or the wire mesh.

In general, the patterned fibre web formed in step c) or the fibre web formed in step c1) has a content of fibres, preferably biocompatible fibres, in an amount ranging from 10 to 80 wt.-%, based on the total weight of the patterned fibre web formed in step c) or the fibre web formed in step c1). Preferably, the patterned fibre web formed in step c) or the fibre web formed in step c1) has a content of fibres, preferably biocompatible fibres, in an amount ranging from 12 to 70 wt.-%, more preferably from 15 to 65 wt.-% and most preferably from 18 to 60 wt.-%, based on the total weight of the patterned fibre web formed in step c) or the fibre web formed in step c1). Additionally or alternatively, the patterned fibre web formed in step c) or the fibre web formed in step c1) has a solvent content, e.g. water, ranging from 20 to 90 wt.-%, based on the total weight of the patterned fibre web formed in step c) or the fibre web formed in step c1). Preferably, the patterned fibre web formed in step c) or the fibre web formed in step c1) has a solvent content, e.g. water, ranging from 30 to 88 wt.-%, more preferably from 35 to 85 wt.-% and most preferably from 40 to 82 wt.-%, based on the total weight of the patterned fibre web formed in step c) or the fibre web formed in step c1).

According to step d) of the present invention, the patterned fibre web is dried to obtain the crease patterned fibre article.

Drying step d) can be carried out by any means known to the skilled person for decreasing the moisture content in a fibre web.

For example, drying step d) is carried out under vacuum or partial vacuum.

Additionally or alternatively, drying step d) is carried out at a temperature ranging from 80 to 200° C., preferably from 85 to 180° C. and most preferably from 90 to 150° C.

In one embodiment, drying step d) is carried out under vacuum (or partial vacuum) or a temperature ranging from 80 to 200° C., preferably from 85 to 180° C. and most preferably from 90 to 150° C. Preferably, drying step d) is carried out under vacuum (or partial vacuum) and a temperature ranging from 80 to 200° C., preferably from 85 to 180° C. and most preferably from 90 to 150° C.

The crease patterned fibre article is thus a dried crease patterned fibre article. The dried crease patterned fibre article preferably has a moisture content of ≤12 wt.-%, more preferably of ≤11 wt.-% and most preferably of ≤10 wt.-%, based on the total weight of the crease patterned fibre article. For example, the dried crease patterned fibre article has a moisture content ranging from 0.5 to 12 wt.-%, more preferably from 0.8 to 11 wt.-% and most preferably from 1 to 10 wt.-%, based on the total weight of the crease patterned fibre article.

It is preferred that the (dried) crease patterned fibre article is separated from the crease patterning device.

The method of the present invention thus preferably comprises a further step e) of separating the crease patterned fibre article from the crease patterning device.

The method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article, and
  • e) separating the crease patterned fibre article from the crease patterning device.

In case of the alternative method, the (dried) crease patterned fibre article is separated from the crease patterning device and wire mesh.

The alternative method of the present invention thus preferably comprises a further step e) of separating the crease patterned fibre article from the crease patterning device and wire mesh.

The method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article, and
  • e) separating the crease patterned fibre article from the crease patterning device and wire mesh.

It is preferred that the (dried) crease patterned fibre article is folded into a desired 3D shape. Such folding can be done by any method known by the skilled person. The folding is done along the creases of the crease patterned fibre article.

The method of the present invention thus preferably comprises a further step f) of folding the crease patterned fibre article into a 3D shape.

The method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) separating the crease patterned fibre article from the crease patterning device, and
  • f) folding the crease patterned fibre article into a 3D shape.

The alternative method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) separating the crease patterned fibre article from the crease patterning device and wire mesh, and
  • f) folding the crease patterned fibre article into a 3D shape.

In one embodiment, the alternative method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article, and
  • f) folding the crease patterned fibre article into a 3D shape.

It is appreciated that the crease patterned fibre article may be used as a scaffold for living cells to potentially substitute animal trials. In particular, the scaffold is thus a tissue scaffold such as for cardiovascular cells, e.g. endothelial cells, vascular smooth muscle cells, lymphatic endothelial cells, cardiomyocytes, and atherosclerosis cells, or skin cells, e.g. keratinocytes, melanocytes, Langerhans cells, and Merkel cells, or bone cells, e.g. osteoblasts, osteocytes, osteoclasts, and osteoprogenitor cells. The crease patterned fibre article may be also used as bio-tissue implant, organ substitute, organ regeneration (patch), tissue substitute or bone reinforcement. In such embodiments, it may be advantageous if the crease patterned fibre article comprises cells and/or enzymes and/or pharmaceuticals to support the function of the article.

The method of the present invention thus preferably comprises a further step g) of applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article.

The method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) separating the crease patterned fibre article from the crease patterning device,
  • f) folding the crease patterned fibre article into a 3D shape, and
  • g) applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article.

The alternative method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) separating the crease patterned fibre article from the crease patterning device and wire mesh,
  • f) folding the crease patterned fibre article into a 3D shape, and
  • g) applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article.

For example, the method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) separating the crease patterned fibre article from the crease patterning device,
  • f) folding the crease patterned fibre article into a 3D shape, and
  • g) applying enzymes onto at least one side of the crease patterned fibre article.

The alternative method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, thus preferably comprises the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web,
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) separating the crease patterned fibre article from the crease patterning device and wire mesh,
  • f) folding the crease patterned fibre article into a 3D shape, and
  • g) applying enzymes onto at least one side of the crease patterned fibre article.

It is further to be noted that a patterned fibre article onto which cells and/or enzymes and/or pharmaceuticals are applied is typically sterilized before step g) of applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article is carried out.

It is appreciated that the cells and/or enzymes and/or pharmaceuticals are preferably applied in a carrier material. The carrier material can be any material known to be suitable for the intended use. For example, the carrier material is selected from the group comprising gelatin, methylcellulose, alginate, agarose, fibrin, hyaluronic acid, K-carrageenan, poly(ethylene glycol) (PEG), polycaprolactone (PCL), matrigel, gelatin methacrylate, poloxamer, nanocellulose, peptide, silk fibroin and mixtures thereof.

Thus, it may be necessary to apply a further step of drying the crease patterned fibre article onto which the cells and/or enzymes and/or pharmaceuticals are applied in order to harden the carrier material. Such further step of drying is preferably carried out at under vacuum or partial vacuum.

Additionally or alternatively, such further step of drying is carried out at a temperature ranging from 30 to 200° C., preferably from 35 to 180° C. and most preferably from 40 to 150° C.

In one embodiment, such further step of drying is carried out under vacuum (or partial vacuum) or a temperature ranging from 30 to 200° C., preferably from 35 to 180° C. and most preferably from 40 to 150° C. Preferably, such further step of drying is carried out under vacuum (or partial vacuum) and a temperature ranging from 30 to 200° C., preferably from 35 to 180° C. and most preferably from 40 to 150° C.

It is to be noted that enzymes can be used as crosslinker for cells supplements in a gelatin matrix, which will make the gelatin permanently. In one embodiment, step g) thus includes applying cells and enzymes onto at least one side of the crease patterned fibre article. In this embodiment, it is further appreciated that the carrier material is preferably gelatin. For example, the enzyme used for crosslinking the carrier material, for example gelatin, is transglutaminase enzyme. Preferably, the enzyme is used in amounts typically applied for crosslinking the carrier material used. For example, the enzyme is used in an amount ranging from 0.01 to 30 vol.-%, based on the total amount of the carrier material, preferably from 0.05 to 20 vol.-% and most preferably from 0.1 to 15 vol.-%.

In one embodiment, the carrier material is gelatin and the enzyme is transglutaminase enzyme.

The pharmaceuticals that are applied onto at least one side of the crease patterned fibre article are preferably selected from grow factors, adhesion proteins, chemotherapeutics, vaccines such as mRNA vaccines, proteins such as spike proteins, cell culture serum, peptides, antibiotics, anti-inflammatory drugs, biomarkers and the like.

It is appreciated that the method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, may comprise a further step of cross-linking the carrier material in which cells and/or enzymes and/or pharmaceuticals are applied. Such step may be advantageous in order to further immobilize the crease patterned fibre article, preferably the crease patterned paper or paperboard. Such cross-linking of the carrier material can be carried out by using any cross-linking agent that is known for cross-linking the corresponding carrier material, provided that the carrier material is suitable to be cross-linked.*

In one embodiment, the method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, comprises a further step of cross-linking the carrier material in which enzymes are applied.

For example, the cross-linking, depending on the carrier material, can be carried out by using UV radiation (e.g. for the carrier material gelatin methacrylate) or thermal crosslinking (e.g. for the carrier material matrigel and poloxamer) or enzymes (e.g. for the carrier material gelatin). Other suitable methods for cross-linking may use agents selected from calcium chloride, potassium chloride and the like.

In one embodiment, the cross-linking, depending on the carrier material, is carried out by using transglutaminase enzymes. For example, the cross-linking of gelatin as carrier material is carried out by using transglutaminase enzymes.

In case cells are applied on the crease patterned fibre article, it is appreciated that such further step of cross-linking is preferably carried out at a temperature ranging from 30 to 100° C., preferably from 35 to 60° C. and most preferably from 35 to 50° C.

It is further preferred that the further step of cross-linking is carried out at high relative humidity. For example, at a relative humidity of at least 90%, preferably from 90 to 98%, most preferably from 92 to 97%. Additionally or alternatively, the further step of cross-linking is carried out in an atmosphere comprising from 3 to 6 vol.-% CO₂. Additionally or alternatively, the further step of cross-linking is carried out for at least 10 min and/or at most 2 hours. For example, the further step of cross-linking is carried out for 10 min to 2 hours, preferably for 20 min to 90 min and most preferably for 20 min to 60 min.

In view of the results obtained, the present invention refers in another aspect to a crease patterned fibre article, preferably a crease patterned paper or paperboard, obtainable by the method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, as defined herein.

Thus, the crease patterned fibre article is obtainable by a method comprising the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) optionally separating the crease patterned fibre article from the crease patterning device,
  • f) optionally folding the crease patterned fibre article into a 3D shape, and
  • g) optionally applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article.

Alternatively, the crease patterned fibre article, preferably a crease patterned paper or paperboard, is obtainable by a method comprising the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) optionally separating the crease patterned fibre article from the crease patterning device and wire mesh,
  • f) optionally folding the crease patterned fibre article into a 3D shape, and
  • g) optionally applying cells and/or enzymes and/or pharmaceuticals onto at least one side of the crease patterned fibre article.

In one embodiment, the crease patterned fibre article is obtainable by a method comprising the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto one surface of the crease patterning device and filtrating the aqueous suspension to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) optionally separating the crease patterned fibre article from the crease patterning device,
  • f) optionally folding the crease patterned fibre article into a 3D shape, and
  • g) applying enzymes onto at least one side of the crease patterned fibre article.

Alternatively, the crease patterned fibre article, preferably a crease patterned paper or paperboard, is obtainable by a method comprising the steps of:

• • a) providing a crease patterning device,
  • b) providing an aqueous suspension comprising fibres, preferably biocompatible fibres,
  • c1) depositing the aqueous suspension comprising fibres, preferably biocompatible fibres, onto a wire mesh and filtrating the aqueous suspension to form a fibre web,
  • c2) patterning the fibre web by using a crease patterning device to form a patterned fibre web, and
  • d) drying the patterned fibre web to obtain the crease patterned fibre article,
  • e) optionally separating the crease patterned fibre article from the crease patterning device and wire mesh,
  • f) optionally folding the crease patterned fibre article into a 3D shape, and
  • g) applying enzymes onto at least one side of the crease patterned fibre article.

With regard to the definition of the method for preparing a crease patterned fibre article and preferred embodiments thereof, reference is made to the statements provided above when discussing the technical details of the methods of the present invention.

In view of the above, it is appreciated that the crease patterned fibre article, preferably the crease patterned paper or paperboard, is preferably a folded crease patterned fibre article, preferably a folded crease patterned paper or paperboard. That is to say, in this embodiment, the crease patterned fibre article, preferably a crease patterned paper or paperboard, i.e. the folded crease patterned fibre article, preferably the folded crease patterned paper or paperboard, is a 3D crease patterned fibre article, preferably a 3D crease patterned paper or paperboard.

It is preferred that the crease patterned fibre article, preferably the crease patterned paper or paperboard, has a paper weight ranging from 10 to 90 g/m², preferably from 10 to 70 g/m², and most preferably from 20 to 60 g/m². For example, the crease patterned fibre article, preferably the crease patterned paper or paperboard, has a paper weight ranging from 30 to 50 g/m², e.g. about 40 g/m².

It is to be noted that the crease patterned fibre article is not particularly limited. However, it is preferred that the crease patterned fibre article is a packaging, design article, fabrics, bio-tissue implant, organ substitute, organ regeneration (patch), organ model, tissue substitute, tissue model, tissue scaffolds, cell growth support, cell maturing support or bone reinforcement.

According to another aspect of the present invention, it is referred to the use of a crease patterned fibre article as a packaging, design article, fabrics, bio-tissue implant, organ substitute, organ regeneration (patch), organ model, tissue substitute, tissue model, tissue scaffolds, cell growth support, cell maturing support or bone reinforcement.

The creased patterned fibre article is preferably obtainable by the method for preparing a crease patterned fibre article, preferably a crease patterned paper or paperboard, as defined herein.

With regard to the definition of the method for preparing a crease patterned fibre article and preferred embodiments thereof, reference is made to the statements provided above when discussing the technical details of the methods of the present invention.

BRIEF DESCRIPTION OF THE FIGURES

FIG. 1 shows the polymer moulds and pressure device used to deform the wire mesh

FIG. 2 shows the resulting crease patterned paper

FIG. 3 shows a copper wire that was used to create the wire Yoshimura pattern

FIG. 4 shows a dried and folded sample

FIG. 5 shows the mould made of PC

FIG. 6 shows the depositing of the mould on top of the wet paper

FIG. 7 shows the wet paper having the stamp of the mould

FIG. 8 shows the positive and negative PLA moulds with the Miura pattern

FIG. 9 shows the paper with the Miura pattern in the top (9A) and cross sectional view (9B).

The scope and interest of the invention will be better understood based on the following examples which are intended to illustrate certain embodiments of the present invention and are non-limitative.

EXAMPLES

1. Equipment

The following equipment as used for the present examples:

	Stirrer	Janke & Kunkel IKA-
		Labortechnik RW 28 W
	Sheet former	Rapid Köthen; Gerd Senkel 110.159
	Sheet Press	PTI Modell 40140 Serien Nr. 0927
	Speed dryer	Lorentzen & Wettrer Rapid Dryer #778

Mechanical press

	3D printer	Ultimaker S5
	3D printer	Formlabs 3B

2. Material

• • Cotton linters/CPW 90 with refining 5.4 KW/45 sec, Supplied by papiertechnische Stiftung (PTS).
  • Eucalyptus fibres of 12 μm in diameter and 0.9 mm length, supplied by Fibria
  • Wire steel mesh: wire 60 warp wire/cm; 55 weft wire/cm; wire-diameter 0.060-0.065 mm,
  • 3D printed moulds made of DentalSG, “The material is a Class I biocompatible resin (EN ISO 10993-1:2021-05)”
  • 3D printed moulds made of PLA
  • 3D printed moulds made of PC
  • copper wire flies & more 0.18 mm, Bernhard fishing CH

3. Paper Elaboration

For all the examples, the fibres were collected as described in this section. The variations on the process are explained in each example.

The fibres were suspended and hydrated at room temperature in 4 L of tap water in a plastic container of 6 L. The fibres were stirred for 10 min at 540 rpm. After stirring, the fibres were placed in a mixer container and were diluted with tap water to 5 L total volume. The fibre slurry was stirred constantly at 140 rpm.

The elaboration of the sheet papers were performed according ISO 5269-2 norm on a Rapid Köthen sheet former. From the fibre slurry the desired amount was taken to form dry sheets of 40 g/m². The fibres were further water suspended and diluted in the cylindrical vessel of the Rapid Köthen until a final volume of 6 L. The fibres were agitated using air-bubbles coming from the bottom of the column for 5 s followed by a vacuum dewatering step. The fibres which were distributed on the bottom of the apparatus and collected by the metallic wire mesh (steel top wire mesh supported by a bronze supported screen) were dried. The drying step is explained in each of the following examples.

EXAMPLES

Example 1. Embossing of the Wire Steel Mesh

The wire steel mesh was slowly pressed in between the positive and negative 3D printed polymer moulds, made previously in a Formalabs 3D printer with Dental SG material. Polymer moulds and pressure device used to deform the wire mesh are shown in FIG. 1.

The wire was used as the base wire for the elaboration of the paper on the Rapid Köthen. The wet paper mounted on the wire was put in the oven at 120° C. for 15 minutes.

The dry sheet of 40 g/m² with the crease (Miura) pattern was carefully removed from the wire mesh. FIG. 2 shows the resulting crease patterned paper.

Example 2. Mark on Paper Via Wire Pattern on the Wire Steel Mesh

To create a wire pattern on the Rapid Köthen wire mesh the Yoshimura pattern, retrieved with Google, was printed out on paper. This paper was used as a template to puncture holes at the pattern nodes into the mesh by means of a stitching awl. Then, a copper wire was used to weave the pattern by pushing the wire through the punched holes and tightening to create the wire pattern as shown in FIG. 3.

The wire mesh with the pattern was then used for paper forming on the Rapid Köthen. The obtained sheet of 40 g/m² was couched to a supporting paperboard and oven dried at 90° C. The dried and folded sample is shown in FIG. 4.

Example 3. 2D Crease Pattern and/or 3D Crease Pattern on Paper

1. Mark on Wet Paper Via Pressure

The mould was printed on the ultimarker S5 printer with PC polymer and is shown in FIG. 5. The PC mould provided a Miura pattern.

The wet paper made previously on the Rapid Köthen was transferred to a wet mat and the before mentioned mould was deposited on top of the wet paper as shown in FIG. 6. The mould was pressed on the wet paper at 5 bars on the sheet press. The wet paper had the stamp of the mould, i.e. a 2D (Miura) crease pattern, as shown in FIG. 7. The paper obtained after drying is 40 g/m². Posterior to this step the paper was folded via positive and negative moulds and the 3D crease pattern was formed.

2. Mark and/or 3D Pattern on Wet Paper Via Press and Drying Step

The sample was pressed as described in numeral one. The wet pressed paper and mould were together transferred to the sheet drying section. Posterior to the drying process, the paper was folded via positive and negative moulds and the 3D crease pattern was formed.

In another example, instead of having a 2D mould, a 3D mould was replaced on the pressed and drying section and a 3D crease paper was obtained directly.

Example 4. Embossing of Paper with Positive and Negative Moulds

PLA positive and negative moulds with the Miura pattern were 3D printed on the Ultimaker S5 (shown in FIG. 8).

The pattern was transferred to the paper on an already formed wetted paper. The process consisted of putting the paper between the two moulds and start slowly the pressure of the moulds until both positive and negative moulds were aligned and together. After this, the paper was dried at 100° C. for 15 min in the oven. The paper with the Miura pattern is shown in FIGS. 9A and B (cross section area of the 3D crease patterned paper).

Example 5. 3D Crease Patterning on Paper

1. Paper Formation

The fibre materials listed in Table 1 were used to produce the creased patterned paper.

TABLE 1
Cellulose fibre materials composition and fibre dimensions

		Fibre		Measured
		average	Fibre	method
Sample	Cellulose fibre	diameter	length	provided by
No	composition	(μm)	(mm)	supplier	Supplier

1	Eucalyptus 100%	12	0.9	Fiber image	Fibria
				analyzerFS5
2	Pine 20-30%, spruce	30	2.4-2.6	Kajaani MAP	Mercer
	70-80% (NBSK)				Pulp
3	Lodgepole pine 50-60%,	28-29	2.51	Kajaani FS200	Canfor
	White spruce 30-40%,
	sub-alpine fir 5-10%
	(NBSK)
	Other 0-10%
4	Pine 70-100%,	23.75	1.8	Kajaani FSA	Metsä
	spruce 0-30%
5	Cotton linters 100%	18 ± 6.2	3 ± 0.9	Length stereo	Research
				microscope	purpose
				reflected light
				ring light, width
				transmitted light
				brightfield*
6	10 wt % Lyocell fiber	12	10	Controlled	Lenzing
	produce by a solvent			process
	spinning process. Raw
	material used is wood
	pulp derived from
	eucalyptus, pine and
	beech trees.
	90 wt % Sample 2
*Measurements performed under optical inspection in 10 samples

Papers were mainly produced using a Rapid Köthen sheet former from Gerd Senkel and a dynamic sheet former (DSF) from CanPa. The Rapid Köthen system triggers a typical stochastic distribution of the fibers in normal use, whereas the DSF can be employed to induce fiber alignment by means of a rotational mesh in the form of a cylinder. For both methods paper sheets of 40 g/m² were produced. Conditions of each method are as follows:

• • Rapid Köthen sheet former: ISO 5269-2 norm was employed for the paper sheet production. Waterborne diluted fibres (40 g/L) were suspended in a cylindrical vessel and filled up until the final volume of 6 liters with water. The fibres were agitated using air-bubbling through the vessel for 5 s followed by dewatering by vacuum. The fibres which were distributed on the bottom of the apparatus and collected by a metallic wire mesh (bronze top mesh supported by steel grid) into a wet mat, were transferred to a carrier board for further dewatering and drying.
  • Dynamic sheet former: A suspension of 0.23 wt % of solid content made with fibres and water was sprayed with a flow rate of 9.9 L/min on a rotatory cylindrical mesh with a speed of 1400 min−1. The excess of water was removed by centrifugal forces. The formed sheet was transferred to a carrier board where the wire was removed and the formed sheet was dewatered and dried. The formed sheet was dewatered twice using pressure and it was dried in a drum drier at 60° C.

The mechanical properties in MD and CD were first evaluated for the dry papers. All samples were measured under controlled conditions (50% RH and 23° C.) according to the ISO 187 norm. The grammage was measured using an analytical balance according to the ISO 536 norm. The thickness of the papers was measured with a Lorentzen & Wettre micrometer according with the EN ISO 12625-3 norm. The specimen dimensions for the samples elaborated with the Rapid Köthen and DSF were 15 mm of width×150 mm of length (clamping length 100 mm). For each measurement 10 specimens were evaluated in a Lorentzen & Wettre tensile tester using a speed for the tensile test of 10 mm/min. DSF sheets were evaluated in MD and CD while the samples produced with the Rapid Köthen were evaluated in random direction.

Table 2 shows the values of strain at break, tensile strength and E-Modulus for each of the assessed paper sheets.

TABLE 2
Mechanical properties of papers produced with the Rapid Köthen

		Strain at	Tensile	E-Modulus
	Sample No	break (%)	strength(MPa)	(Gpa)

	1	1.0 ± 0.2	13.4	2.8 ± 0.2
	2	1.3 ± 0.2	9.1	1.8 ± 0.2
	3	1.8 ± 0.1	20.6	3.4 ± 0.5
	4	1.5 ± 0.1	17.9	3.0 ± 0.4
	5	1.3 ± 0.1	4.7	0.8 ± 0.1
	6	2.3 ± 0.2	35.0	4.4 ± 0.2

The wide range of breaking strength (1-2.3%), tensile strength (4.7-35 MPa) values and the high E-modulus (0.8-4.4 GPa) demonstrate the versatility of the papers prepared.

2. 3D Origami Pattern Transfer

Two following methods were used to generate the 3D origami crease pattern on the paper.

Method A, dry embossing: Two 75 μm thick PET foils were thermoplastically deformed (T=80° C., P=100 g/cm², t=1 h) into the Miura pattern, by pressing between two previously 3D printed stamps (Formlabs, DentalSG). The paper was sandwiched between the two Miura's patterned PET preforms and the sandwich was folded and unfolded by hand allowing desired pattern to be transferred onto the paper. The folding and unfolding of the foil-paper-foil sandwich allowed the paper to slide in place during the folding process and avoid tearing the paper apart as would have been the case when embossing with rigid stamps.

Method B: wet forming: The origami pattern was generated in-situ during the wet paper forming process onto a wire mesh containing the origami crease pattern in the paper-sheet former's draining section. Two approaches were used to produce the patterned wire mesh: The first variant employs a 3D printed origami shaped mesh (DentalSG, Formlabs) which was mounted on top of a standard wire mesh. In the second approach, the 3D pattern was embossed into a standard wire mesh using 3D patterned stamps similar to the one used in method A. The sieved paper was dried on the modified mesh in the oven for 15 min at 120° C. Thereafter the patterned paper was removed from the wire mesh.

3. Immobilization of the Crease Patterned Paper

The structural stability of the crease patterned paper was fixed by the addition of hydrogel. The crease patterned and folded papers were mounted on a 3D printed form with the same origami pattern and wetted with 20 μl of 10% w/v gelatin (Porcine skin, Sigma Aldrich) solution including 1% v/v transglutaminase enzyme. The assembly was allowed to enzymatically crosslink in a conventional cell culture incubator at 37° C. 5% CO₂ and 95% RH for 30 minutes.

The mechanical properties of immobilized crease patterned papers were assessed in wet conditions. For each material, five wetted specimens were measured under the same room, machine conditions and specimen size described above (see item 2). Tensile strength was calculated from the measured data (tensile force/initial width of the specimen).

The tensile strength in wet conditions for sample 2 and 5 were 3.74 and 2.28 (MPa), respectively. This suggests that the immobilized crease patterned paper could work for tissue engineering applications.