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EP3046755A1 - Surfaces imprégnées d'un liquide non toxique - Google Patents

Surfaces imprégnées d'un liquide non toxique

Info

Publication number
EP3046755A1
EP3046755A1 EP14844341.9A EP14844341A EP3046755A1 EP 3046755 A1 EP3046755 A1 EP 3046755A1 EP 14844341 A EP14844341 A EP 14844341A EP 3046755 A1 EP3046755 A1 EP 3046755A1
Authority
EP
European Patent Office
Prior art keywords
liquid
features
solid
impregnating liquid
impregnated
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP14844341.9A
Other languages
German (de)
English (en)
Other versions
EP3046755A4 (fr
Inventor
J. David Smith
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Liquiglide Inc
Original Assignee
Liquiglide Inc
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Liquiglide Inc filed Critical Liquiglide Inc
Publication of EP3046755A1 publication Critical patent/EP3046755A1/fr
Publication of EP3046755A4 publication Critical patent/EP3046755A4/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B65—CONVEYING; PACKING; STORING; HANDLING THIN OR FILAMENTARY MATERIAL
    • B65D—CONTAINERS FOR STORAGE OR TRANSPORT OF ARTICLES OR MATERIALS, e.g. BAGS, BARRELS, BOTTLES, BOXES, CANS, CARTONS, CRATES, DRUMS, JARS, TANKS, HOPPERS, FORWARDING CONTAINERS; ACCESSORIES, CLOSURES, OR FITTINGS THEREFOR; PACKAGING ELEMENTS; PACKAGES
    • B65D85/00—Containers, packaging elements or packages, specially adapted for particular articles or materials
    • B65D85/70—Containers, packaging elements or packages, specially adapted for particular articles or materials for materials not otherwise provided for
    • B65D85/72—Containers, packaging elements or packages, specially adapted for particular articles or materials for materials not otherwise provided for for edible or potable liquids, semiliquids, or plastic or pasty materials
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B65—CONVEYING; PACKING; STORING; HANDLING THIN OR FILAMENTARY MATERIAL
    • B65D—CONTAINERS FOR STORAGE OR TRANSPORT OF ARTICLES OR MATERIALS, e.g. BAGS, BARRELS, BOTTLES, BOXES, CANS, CARTONS, CRATES, DRUMS, JARS, TANKS, HOPPERS, FORWARDING CONTAINERS; ACCESSORIES, CLOSURES, OR FITTINGS THEREFOR; PACKAGING ELEMENTS; PACKAGES
    • B65D23/00—Details of bottles or jars not otherwise provided for
    • B65D23/02—Linings or internal coatings
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B65—CONVEYING; PACKING; STORING; HANDLING THIN OR FILAMENTARY MATERIAL
    • B65D—CONTAINERS FOR STORAGE OR TRANSPORT OF ARTICLES OR MATERIALS, e.g. BAGS, BARRELS, BOTTLES, BOXES, CANS, CARTONS, CRATES, DRUMS, JARS, TANKS, HOPPERS, FORWARDING CONTAINERS; ACCESSORIES, CLOSURES, OR FITTINGS THEREFOR; PACKAGING ELEMENTS; PACKAGES
    • B65D25/00—Details of other kinds or types of rigid or semi-rigid containers
    • B65D25/14—Linings or internal coatings

Definitions

  • micro/nano-engineered surfaces in the last decade has opened up new techniques for enhancing a wide variety of physical phenomena in themiofiuids sciences.
  • the use of micro/nano surface textures has provided non-wetting surfaces capable of achieving less viscous drag, reduced adhesion to ice and other materials, self-cleaning, water repeilency, and other useful properties. These improvements result generally from diminished contact (i.e., less wetting) between the solid surfaces, and adjacent liquids.
  • One type of non-wetting surface of interest is a super hydrophobic surface.
  • a super hydrophobic surface includes micro/nano-scale roughness on an intrinsically hydrophobic surface, such as a hydrophobic coating. Super hydrophobic surfaces resist contact with water by virtue of an air-water interface within the micro/nano surface textures.
  • non-wetting surfaces e.g., superhydrophobic, superoleophobic, and supermetallophobic surfaces
  • they are susceptible to evaporation and partial entrainment of constituents therein (e.g., in the presence of water and/or a product in contact with the surface), which can degrade the hydrophobicity, and in a consumer products context may lead to concerns about materials toxicity (i.e., as they degrade and/or dissociate).
  • materials toxicity i.e., as they degrade and/or dissociate.
  • Embodiments described herein relate generally to containers having liquid- impregnated surfaces disposed on their interior surfaces.
  • the liquid-impregnated surfaces may compose an arrangement of solid and/or semi-solid features, defining one or more interstitial regions therebetween, and an impregnating liquid preferentially wetted to those regions.
  • the containers may be designed to contain a product that is intended for human or animal consumption.
  • the solid and/or semi-solid features and the impregnating liquid collectively define a secondary surface (e.g., substantially parallel to the interior surface on which the liquid-impregnated surfaces are disposed) and may include materials which are non-toxic.
  • non-toxic liquid- impregnated surfaces of the disclosure may be configured for use in food, drug, health and/or beauty product applications, and industrial applications where people make contact with the coating materials, or where fumes or vapors in the manufacturing of coating materials or products made in the industrial applications poses a safety concerns for workers.
  • the interstitial regions are dimensioned and configured such that the impregnating liquid is retained within the interstitial regions by capillary forces.
  • the impregnating liquid disposed in the interstitial regions and the solid features collectively defines a secondary surface having a second roil off angle less than a first roll off angle of the initial/interior surface.
  • the liquid-impregnated surface in use, is in contact with at least one of a food product, drug, or health and beauty product, and the impregnatmg liquid included in the liquid-impregnated surface is non-toxic.
  • the solid features included in the liquid-impregnated surface can also be formed from materials that are nontoxic.
  • at least one of the impregnating liquid and the solid features included in the l quid-impregnated surface can include: materials that are approved by the U.S. Food and Drug Administration (FDA) for use as a food additive, an FDA approved food contact substance, an FDA "General!' Regarded as Safe” (GRAS) material, an FDA approved drug ingredient, and/or or an FDA approved health and beauty product ingredient.
  • FDA U.S. Food and Drug Administration
  • FIG. 1A is a schematic cross-section view of a product contacting a conventional super-hydrophobic surface
  • FIG. IB shows the conventional non-wetting surface after a product has impaled the surface.
  • FIG. 2 shows a schematic cross-section of a liquid-impregnated surface according to an embodiment.
  • FIG. 3 is a scanning electron microscope (SEM) micrograph of a surface including semi-solid features according, to an embodiment.
  • FIG. 4 is a SEM micrograph of a surface including hierarchical semi-solid features, according to an embodiment.
  • FIG. 5 is a SEM micrograph of the surface of FIG. 3 partial!)' impregnated with an impregnating liquid.
  • FIG. 6 is an enlarged higher-magnification view of the region of the liquid- impregnated surface indicated by arrow A in FIG. 5.
  • FIGS. 7A and 7B are schematic diagrams of liquid droplets placed on a liquid- impregnated surfaces (having a low surface energy lubricant, and a having moderate surface energy lubricant, respectively) according to an embodiment.
  • FIGS. 7C and 7D show photographs of water droplets on the liquid-impregnated surfaces of FIGS. 7A and 7B, respectively.
  • FIGS, 7E and 7F are photographs of water droplets on the liquid-impregnated surfaces of FIGS. 7A and 7B, taken under a fluorescent light, where the liquid includes a fluorescent dye.
  • FIGS. 7G and 7H are LCFM images of liquid-impregnated surfaces (having a low surface energy lubricant, and a having moderate surface energy lubricant, respectively) according to an embodiment.
  • FIGS. 71 and 7J are environmental scanning electron microscope (ESEM) images of liquid-impregnated surfaces (having a low surface energy lubricant, and a having moderate surface energy lubricant, respectively) according to an embodiment.
  • ESEM environmental scanning electron microscope
  • FIG. 8 is a table of schematics and characteristic equations for wetting surface configurations having an oil-solid-air interface (top three rows) and at an oil-solid-water interface (bottom three rows), where the subscript "o" denotes the impregnating liquid (e.g. oil).
  • the impregnating liquid e.g. oil
  • FIG. 9 shows possible thermodynamic states of a water droplet (or other external phase) on liquid-impregnated surfaces.
  • FIG. 10A is a plot of measured roll off angles for liquid-impregnated surfaces, according to an embodiment.
  • FIG. 10B is a SEM image of a liquid-impregnated surface with solid features, according to an embodiment.
  • FIG. IOC is a SEM image of a liquid-impregnated surface having hierarchical solid features, according to an embodiment.
  • FIG. 10D is a non-dimensional plot of scaled gravitational force at the instant of roll-off, as a function of the relevant pinning force of the liquid-impregnated and non- impregnated surfaces of FIG. 9.
  • FIG. 1 1 A is a plot of measured velocities of water droplets as a function of substrate tilt angle, according to an embodiment.
  • FIG. LI B shows a schematic of a liquid droplet moving on a lubricant- impregnated surface, showing the various parameters considered in the scaling model, according to an embodiment.
  • FIG, I IC shows trajectories of a number of coffee particles measured relative to a water droplet on a liquid-impregnated surface, according to an embodiment.
  • FIG. 11 D shows a non-dimensional plot obtained from a model described herein.
  • FIG. 12 shows a SEM micrograph (at 500X magnification) of a textured substrate formed by spraying a mixture of 0.5 grams carnauba wax and 40 ml ethanoi onto a substrate, according to an embodiment.
  • FIG. 13 is a higher-magnification (15,00GX) SEM micrograph of the textured substrate shown in FIG. 12.
  • FIG. 14 shows a scanning electron microscope (SEM) micrograph of a textured substrate formed by spraying a mixture of 4 grams carnauba wax and 40 ml ethanoi onto a substrate, according to an embodiment.
  • FIG. 15 is a higher-magnification (15,000X) SEM micrograph of the textured substrate shown in FIG. 14.
  • FIG. 16 is a SEM micrograph (at 500X magnification) of a textured substrate formed by spraying an aerosol wax on a substrate, according to an embodiment.
  • FIG. 17 is a higher-magnification (15,00QX) SEM micrograph of the textured substrate shown in FIG, 16.
  • FIGS. 18-23 are a sequence of images of a volume of ketchup disposed on a liquid impregnated surface that includes aerosol wax as the solid and ethyl oleate as the impregnating liquid, such that the volume of ketchup slides on the liquid impregnated surface as the liquid impregnated surface is inclined at an angle.
  • Embodiments described herein relate generally to containers having liquid- impregnated surfaces disposed on their interior surfaces.
  • the liquid-impregnated surfaces may compose an arrangement of solid and/or semi-solid features, defining one or more interstitial regions therebetween, and an impregnating liquid preferentially wetted to those regions.
  • the containers may be designed to contain a product that is intended for human or animal use and/or consumption.
  • the solid and/or semi-solid features and the impregnating liquid collectively define a secondar surface (e.g., substantially parallel to the interior surface on which the liquid-impregnated surfaces are disposed) and may include materials which are non-toxic, in particular, non-toxic liquid-impregnated surfaces of the disclosure may be configured for use in food, drugs, health and/or beauty product applications.
  • the interstitial regions are dimensioned and configured such that the impregnating liquid is retained within the interstitial regions by capillary forces.
  • the secondary surface may have a second roll off angle less than a first roll off angle of the initial/interior surface.
  • the liquid-impregnated surface in use, is in contact with at least one of a food product, drug, or health and beauty product, and the impregnating liquid included in the liquid-impregnated surface is non-toxic.
  • the solid features included in the liquid-impregnated surface can also be formed from materials that are nontoxic.
  • At least one of the impregnating liquid and the solid features included in the liquid- impregnated surface can include: materials that are approved by the U.S. Food and Drag Administration (FDA) for use as a food additive, an FDA approved food contact substance, an FDA “Generally Regarded as Safe” (GRAS) material, an FDA approved drag ingredient, and/or or an FDA approved health and beauty product ingredient.
  • FDA U.S. Food and Drag Administration
  • GRAS Generally Regarded as Safe
  • hydrophobic surfaces with designed chemistry and roughness possess substantial non- wetting (hydrophobic) properties, which can be extremely useful in a wide variety of commercial and technological applications.
  • hydrophobic surfaces include air pockets trapped within a rmcrotexture or nanotexture of the surface which diminishes the contact angle between such hydrophobic surfaces and a liquid thereon, or example, water, an aqueous liquid, or any other aqueous product. As long as the air pockets are stable, the surface continues to exhibit hydrophobic behavior.
  • Such hydrophobic surfaces that include air pockets, however, present certain limitations including, for example: i) the air pockets can be collapsed by external wetting pressures, ii) the air pockets can diffuse away into the surrounding liquid, iii) the surface can lose robustness upon damage to the texture, iv) the air pockets may be displaced by low surface tension liquids unless special texture design is implemented, and v) condensation or frost nuclei, which can form at the nanoscale throughout " the texture, can completely transform the wetting properties and render the textured surface highly wetting.
  • Non-toxic liquid-impregnated surface coatings described herein include impregnating liquids that are impregnated into a surface that includes an arrangement or "matrix" of solid features defining one or more interstitial regions (i.e., between individual features and/or between groupings of features), such that the interstitial regions include volumes or "pockets" of impregnating liquid.
  • the impregnating liquid is configured to wet the solid surface preferentially, and it adheres to the micro-textured surface with strong capillar ⁇ ' forces, enabling an extremely low roll-off angle of a droplet and/or aqueous solution (referred to as contact liquid) that is in contact with the surface.
  • the roll-off angle of the contact liquid in contact with the surface is about 1 degree.
  • This enables the contact liquid to displace, travel, slide, roll off, etc., with substantial ease on the liquid-impregnated surface. Therefore, the non-toxic liquid-impregnated surfaces described herein, provide certain significant advantages over conventional super hydrophobic surfaces including: (i) low hysteresis, (ii) self cleaning properties, (iii) ability to withstand high drop impact pressure (i.e., are wear resistant), (iv) ability to self heal by capillar ⁇ ' wicking upon damage; (v) ability to enhance condensation; and (vi) in the event of evaporation and/or entrainment, toxicity is avoided due to the non-toxic composition of the materials employed.
  • non-toxic liquid-impregnated surfaces described herein which may include solids and/or impregnating liquids that are non-toxic, can he used in applications requiring contact with a variety of products destined for human use or consumption, such as, for example; (a) food products such as, for example ketchup, catsup, mustard, mayonnaise, syrup, honey, jelly, etc.; (b) drugs, for example Food and Drug Administration (FDA) approved drugs; and (c) consumer products, for example toothpaste, shampoo, conditioner, hair gel, etc.
  • methods described herein can enhance the durability of liquid- impregnated surfaces, such that the surface does not wear, wears more slowly, and/or replenishes itself after single and/or repeated use.
  • the terms “about” and “approximately” generally mean plus or minus 10% of the value stated, for example “about 250 um” would include any value from 225 ⁇ to 275 ⁇ , and “approximately 1,000 ⁇ ” (or “1 mm”) would include any value from 900 ⁇ to 1 ,100 ⁇ .
  • contact liquid and the terms “fluid” and “product” may refer to a solid or liquid that flows, for example a non-Newtonian fluid, a Bingham fluid, or a thixotropic fluid.
  • a “contact liquid” is any such material that is in contact with a liquid- impregnated surface, unless otherwise stated.
  • emerged area fraction also “non-submerged area fraction”
  • ⁇ is defined as a representative fraction of the surface area of a liquid-impregnated surface corresponding with non-submerged solid (i.e., solid that is not covered up by the impregnating liquid, and hence may be in direct contact with an adjacent product material) at room temperature.
  • a conventional non-wetting surface 10 is a textured surface configured such that the non- wetting surface 10 includes a plurality of solid features 12 disposed on the surface 10.
  • the solid features 12 define interstitial regions between each of the plurality of solid features which are impregnated by a gas, for example, air,
  • a product P e.g., a non-Newtonian fluid, a Bingham fluid or a thixotropic fluid
  • the interface 14 is configured such thai- it prevents or delays the product from wetting the entire surface 10.
  • the product P can displace and/or dissolve the impregnating gas and "impales" the interstitial regions between the features 12 of the surface 10 (it may also be said that the product P is "impaled” by the features).
  • Such impalement may occur, for example, when a droplet of the product P impinges the surface 10 at a high velocity.
  • the gas occupying the regions between the solid features 12 is replaced with the product P, either partially or completely, and the surface 10 may lose its non-wetting capabilities as a consequence.
  • a liquid-impregnated surface 130 includes a solid surface 110 that includes a plurality of solid features 1 12 disposed on the solid surface 110 (e.g., the solid features projecting therefrom, adhered thereon/thereto, or comprising projections between recessed regions in the surface, and/or the like) such that the plurality of solid features 1 12 define interstitial regions between each (individual) of the plurality of solid features and/or between clusters of such solid features.
  • An impregnating liquid 120 is "impregnated" (e.g., introduced, pumped, brushed, applied, injected, rolled, sprayed, poured, etc.) into the interstitial regions defined by the plurality of solid features 1 12.
  • a product P is disposed on the liquid-impregnated surface 100 such that a liquid- product interface 124 separates the product P from the surface 1 10 and prevents the product P from entirely wetting the surface 110.
  • the liquid-impregnating surface 130 having a product disposed thereon is collectively indicated by reference numeral 100.
  • the product P can be any product, for example, a non-Newtonian fluid, a
  • the product P can include, for example a food product, a drug, a health and/or beauty product, and/or any other product described herein, or a combination thereof.
  • the surface 110 can be any surface that has a first roll off angle or no roll-off angle (e.g. a really sticky surface), for example a roll off angle of a product in contact with the surface 1 10 (e.g., water, food products, drugs, health or beauty products, or any other products described herein) under a specified environmental condition (e.g., temperature, pressure, etc.).
  • the surface 110 can be a flat surface, for example, a silicon wafer, a plastic sheet stock, a metal sheet stock, a glass wafer, a ceramic substrate, a table top, a wall, a wind shield, a ski goggle screen, etc.
  • the surface 110 can also be a contoured surface, for example a container, a propeller, a pipe, etc.
  • the surface 110 can include an interior surface of a container for housing the product P, and the container may be any of the fol lowing exemplary containers: tube, bottle, hopper, tray, vial, flask, mold, jar, cup, glass, pitcher, barrel, bin, tote, tank, keg, tub, syringe, tin, pouch, box (e.g., a lined box), hose, cylinder, and can (e.g., a tin can).
  • the container can be constructed in almost any desirable shape.
  • the surface 110 can be an interior surface of a hose, a pipe, a conduit, a nozzle, a paint applicator (e.g., a paint sprayer), a syringe needle, a dispensing tip, a lid, a pump, and/or a surface of any other apparatus for containing, transporting, and/or dispensing a product P.
  • the surface 110 for example comprising the interior surface of a container, can be constructed of any suitable material, including plastic, glass, metal (including metal meshes and metallic containers lined with linen), Styrofoam, ceramic, coated fibers, and combinations thereof.
  • Suitable surfaces can also include, for example, polystyrene, nylon, polypropylene, wax, polyethylene terephthalate, polypropylene, polyethylene (e.g., low- density polyethylene, LDPE; high-density polyethylene, HDPE; polyethylene terephthalate, PET), polyurethane, polysuiphone, polyethersulfone, polytetrafluoroethylene (PTFE), tetrafj.uoroethylene (TFE), fluorinated ethylenepropylene copolymer (FEP), polyvinylidene fluoride (PVDF), perfluoroalkoxytetrafluoroethyiene copolymer (PFA), perfluoromethyl vinylether copolymer (MFA), ethylenechlorotrifluoroethylene copolymer (ECTFE), ethylene- tetrafluoroethylene copolymer (ETFE), perfluoropolyether, Tecnoflon cellulose acetate, and polycarbonate
  • the container 1 10 can be constructed of rigid or flexible materials. Foil-lined and polymer-lined cardboard, corrugated, and/or paper boxes can also form suitable containers. In some embodiments, the surface can be solid, smooth, textured, rough, and/or porous.
  • the solid features 1 12 can be disposed on the surface 110 using any suitable method.
  • the solid features 112 can be applied to the inside of a container (e.g., a bottle or other food container), or they can be integral to the surface itself (e.g., the textures of a polycarbonate bottle may be made of polycarbonate).
  • the solid features 112 may be formed of a collection or coating of particles, for example edible solid particles.
  • solid, non-toxic and/or edible materials include (but are not limited to): insoluble fibers (e.g., purified wood cellulose, micro-crystalline cellulose, and/or oat bran fiber), wax (e.g., carnauba wax, japan wax, beeswax, candelilla wax), pulp, zein, dextrin, cellulose, cellulose ethers (e.g., Hydroxyethyl cellulose, Hydroxypropyl cellulose (HPC), Hydroxyethyl methyl cellulose, Hydroxypropyl methyl cellulose (HPMC), Ethyl hydroxyethyl cellulose), ferric oxide, iron oxide, sodium formate, sodium oieate, sodium palmitate, sodium sulfate, gelatin, pectin, gluten, starch alginate, carrageenan, whey and/or any other edible solid particles described herein, or any combination thereof.
  • insoluble fibers e.g., purified wood cellulose, micro-crystalline
  • the solid features may comprise a material having a melting point of about 75°C.
  • the solid features may comprise a material having a melting point of as high as 330°C, as high as 240°C (e.g., for polyurethanes), as high as 60°C, as high as 50°C, between about 40°C and about 50°C.
  • the solid features may comprise a material having a melting point of at least about 60°C.
  • the solid features may comprise a material having a melting point may be as high as about 2,0G0°C.
  • the solid features may comprise materials that are safe for contact with skin, such as a silicone, fluoropolymers (e.g., polytetrafluoroethylene, polychlorotrifluoroethylene, poly(vinylidene difluoride)), nitrile and silicone rubbers, fluorosilicone, poiyurethane, fluoropolyurethane, polyvinylpyrrolidone, fluoroacrylates and halocarbons in general, and their corresponding copolymers with hydrocarbons, silicones, acrylates, meth.acrylat.es, urethanes and other fluoropolymers (e.g.,
  • the solid features may comprise particles including: halocarbons (e.g., polytetrafluoroethylene, polyvinylidene fluoride, chlorotrifluoroethylene, ethylene chlorotrifluoroethylene), ceramics (e.g., surface modified), and metal oxides (e.g., surface modified).
  • halocarbons e.g., polytetrafluoroethylene, polyvinylidene fluoride, chlorotrifluoroethylene, ethylene chlorotrifluoroethylene
  • ceramics e.g., surface modified
  • metal oxides e.g., surface modified
  • the solid features may comprise one or more of the following substances: Japan wax, beeswax, carnauba wax, rice bran wax, a mineral wax, paraffin wax, candelilla wax, zein, shellac, methyl cellulose, stearic acid, cetyl alcohol, stearic alcohol, calcium stearate, zinc stearate, magnesium stearate, titanium oxide, sodium oleate, sodium palmitate, polydimethylsiloxane (PD S), and silicone-based sealant, silicone wax, and silicone-based sealant.
  • materials employed in the formulation of the solid features may have a solubility in an impregnating liquid of the disclosure of not more than 1% (w/w).
  • the solid features 1 12 can be formed by exposing the surface 110 (e.g., polycarbonate) to a solvent (e.g., acetone) (i.e., chemical roughening).
  • a solvent e.g., acetone
  • the solvent may impart texture by inducing crystallization (e.g., polycarbonate may recrystaliize when exposed to acetone).
  • the solid features 112 can be disposed by dissolving, etching, melting, milling, laser rastering, oxidizing (e.g. by boiling in water) and/or evaporating away a portion of a surface, leaving behind a textured, porous, and/or rough surface that includes a plurality of the solid features 112.
  • the solid features 112 can be defined by mechanical roughening (e.g., tumbling with an abrasive or sand-blasting), spray-coating, polymer spinning, deposition of particles from solution (e.g., layer-by-layer deposition, evaporating away liquid from a liquid/particle suspension), and/or extrusion or blow-molding of a foam, or foam-forming material (for example a polyurethane foam).
  • the solid features 1 12 can also be formed by deposition of a polymer from a solution (e.g., the polymer forms a rough, porous, or textured surface); extrusion or blow-molding of a material that expands upon cooling, leaving behind a wrinkled surface; and application of a layer of a material onto a surface that is under tension or compression, and subsequent!)' relaxing the tension or compression of surface beneath, resulting in a textured surface.
  • a polymer from a solution e.g., the polymer forms a rough, porous, or textured surface
  • extrusion or blow-molding of a material that expands upon cooling, leaving behind a wrinkled surface and application of a layer of a material onto a surface that is under tension or compression, and subsequent!' relaxing the tension or compression of surface beneath, resulting in a textured surface.
  • the solid features 112 are formed by non-solvent induced phase separation of a polymer, resulting in a sponge-like porous structure.
  • a solution of polysulfone, poly(vinylpyrrolidone), and dimethylacetamide (DMAc) may be cast onto a substrate and then immersed in a bath of water. Upon immersion in water, the solvent and non-solvent exchange, and the polysulfone precipitates and hardens.
  • the solid features 1 12 may be formed by a self-assembly process, for example the co-deposition of solid and liquid.
  • the self-assembly process may involve the use of molecules such as: alkythiols, alhyldisulfides, alkylselenols, organosilanes, organophosphonates, organophosphates, aikyicarboxilate, among others, for example including different terminal groups configured to modify the chemistry of the surface.
  • the solid features 112 can include micro-scale features such as, for example posts, spheres, nano needles, pores, cavities, interconnected pores, grooves, ridges, interconnected cavities, or any other random geometry that provides a micro and/or nano surface roughness (for example, a roughness averaged over 5 peaks, "S5P," of less than about 25 ⁇ , 10 ⁇ , e.g., 3 ⁇ ), 1 ⁇ , 500 nm.
  • the solid features 112 can include particles that have micro-scale dimensions that can be randomly or uniformly dispersed on a surface.
  • Characteristic spacing between the solid features 112 can be about 200 ⁇ , about 100 ⁇ , about 90 ⁇ , about 80 ⁇ , about 70 ⁇ , about 60 ⁇ , about 50 ⁇ , about 40 ⁇ , about 30 ⁇ , about 20 ⁇ , about 10 um, about 5 ⁇ , between about 2 ⁇ and about 5 ⁇ , about 1 ⁇ , or about 100 nm.
  • the characteristic spacing may be uniform or non-uniform (ordered changes in spacing, linearly varying spacing, random spacing, and/or the like).
  • the spacing is nonuniform provided that the spacing between features on over 99% of the surface does not exceed 200 ⁇ , about 100 ⁇ « ⁇ , about 90 ⁇ , about 80 ⁇ , about 70 ⁇ , about 60 ⁇ , about 50 ⁇ , about 40 ⁇ , about 30 ⁇ , about 20 ⁇ , about 10 ⁇ , about 5 ⁇ , between about 2 ⁇ and about 5 ⁇ , about 1 ⁇ , or about 100 nm.
  • 99% is only important because it means that there are few defect spots where there could be a larger separation between features consequent pinning of the product in those regions.
  • the characteristic spacing between the solid features 112 can be (e.g., on average) in the range of about 100 ⁇ to about 100 nm, about 30 ⁇ to about 1 ⁇ , or about 10 ⁇ to about 1 ⁇ . In some embodiments, characteristic spacing between solid features 112 can be (e.g., on average) in the range of about 100 um to about 80 ⁇ /m, about 80 ⁇ /m to about 50 ⁇ , about 50 ⁇ to about 30 ⁇ , or about 30 ⁇ to about 10 um, inclusive of all ranges therebetween.
  • the solid features 1 12, for example solid “particles,” can have an average dimension (e.g., corresponding to a height, width, diameter, length, and/or the like) of about 200 ⁇ , about 100 ⁇ , about 90 ⁇ , about 80 ⁇ , about 70 ⁇ , about 60 , m, about 50 ⁇ , about 40 ⁇ , about 30 ⁇ , about 20 ⁇ , about 10 um, about 5 ⁇ , about 1 ⁇ , about 0.5 ⁇ , between 0.5 ⁇ and 10 ⁇ , or about 100 nm.
  • an average dimension e.g., corresponding to a height, width, diameter, length, and/or the like
  • the average dimension of the solid features 112 can be in a range of about 100 ⁇ to about 100 um, about 30 ⁇ to about 10 ⁇ , or about 20 ⁇ to about 1 ⁇ . In some embodiments, the average dimension of the solid features 112 can be in a range of about l Onm to about 50 ⁇ . In some embodiments, the average dimension of the solid features 1 12 can be in the range of about 100 ⁇ to about 80 ⁇ , about 80 ⁇ to about 50 ⁇ , about 50 ⁇ to about 30 ⁇ , or about 30 ⁇ to about 10 um, or 10 ⁇ to 100 nm, inclusive of ail ranges therebetween. In some embodiments, the height of the solid features 112 can be substantially uniform. In some embodiments, the surface 1 10 can have hierarchicai features, for example micro-scale features that further include nano-seale features disposed thereupon (e.g., etched therein, adhered thereto, etc.).
  • the solid features 112 can be porous.
  • the characteristic pore size (e.g., pore width or length) of particles can be (e.g., on average) about 5,000 nm, about 3,000 nm, about 2,000 nm, about 1 ,000 nm, about 500 nm, about 400 nm, about 300 nm, about 200 nm, about 100 nm, about 80 nm, about 50, about 10 nm.
  • the characteristic pore size can be in the range of about 200 nm to about 2 ⁇ , or about 50 nm to about 1 ⁇ , inclusive of all ranges therebetween.
  • the impregnating liquid 120 is disposed on the surface 110 such that the impregnating liquid 120 impregnates substantially all of the interstitial regions defined by the plurality of solid features 1 12 (the solid features comprising, for example, pores, cavities, or otherwise inter- feature spacing defined by the surface 110), such that no air remains in the interstitial regions.
  • the interstitial regions can be dimensioned and configured such that capillary forces retain part of the impregnating liquid 120 in the interstitial regions.
  • the impregnating liquid 120 disposed in the interstitial regions of the pluralit of solid features 1 12 is configured such that the liquid-impregnated surface 130 defines a second roll off angle that is less than the first roll of angle (i.e., the roll of angle of the un-impregnated liquid surface 1 10).
  • the impregnating liquid 120 can have a viscosity at room temperature of less than about 1,000 cP, for example about 8 cP, between about I cP and about 10 cP, between about 10 cP and about 20 cP, about 50 cP about 30 cP, between about 8 cP and about 30 cP, about 50 cP, about 80 cP, between about 20 cP and about 100 cP, about 100 cP, between about 100 cP and about 10 P, about 150 cP, about 200 cP, about 300 cP, about 350 cP, about 400 cP, about 500 cP, about 600 cP, about 700 cP, about 800 cP, about 900 cP, between about 10 P and about 100 P, about 1 ,000 cP, or between about 100 P and about 1 ,000 P, inclusive of all ranges therebetween, in some embodiments, the impregnating liquid 120 can have a viscosity of about 8
  • the impregnating liquid 120 can have a viscosity of about 1 ,000 cP or less. In some embodiments, the impregnating liquid 120 can have a vapor pressure at room temperature of less than about 20 mmHg. In some embodiments, the impregnating liquid 120 can have a vapor pressure at room temperature of as low as 4 x 10 " ' mmHg. In some embodiments, the impregnating liquid 120 can have a surface tension of as low as 14 dyn cm. In some embodiments, the impregnating liquid 120 can fill the interstitial regions defined by the solid features 112 and form a layer of at least about 5 nm thick above the plurality of solid features 112 disposed on the surface 1 10.
  • the impregnating liquid 120 forms a layer of at least about 1 ⁇ of excess mobile liquid (easily moved by external forces such as those resulting from shearing or gravity) above the plurality of solid features 1 12 disposed on the surface 110 on some regions of the surface.
  • the impregnating liquid 120 may be disposed in the interstitial spaces defined by the solid features 112 using any suitable means.
  • the impregnating liquid 120 can be sprayed or brushed onto the textured surface 1 10 (e.g., a texture on an inner surface of a bottle).
  • the impregnating liquid 120 can be applied to the textured surface 1 10 by filling or partially filling a container that includes the textured surface 1 10. The excess impregnating liquid 120 is then removed from the container.
  • the excess impregnating liquid 120 can be removed by adding a wash liquid (e.g., water) to the container to collect or extract the excess liquid from the container.
  • a wash liquid e.g., water
  • the excess impregnating liquid may be mechanically removed (e.g., pushed off the surface with a solid object or fluid), absorbed or wicked off of the surface 110 using another porous material, and/or removed via gravity or centrifugal forces.
  • the impregnating liquid 120 can be disposed by spinning the surface 110 (e.g., a container) in contact with the liquid (e.g., a spin coating process), and condensing the impregnating liquid 120 onto the surface 110.
  • the impregnating liquid 120 is applied by depositing a solution comprising the impregnating liquid and one or more volatile liquids (e.g., depositing via any of the previously described methods) and subsequently evaporating away one or more of the volatile liquids.
  • the impregnating liquid 120 can be applied using an external liquid that spreads or pushes the impregnating liquid along the surface 110.
  • the impregnating liquid 120 e.g., ethyl oleate
  • spreading liquid e.g., water
  • the fluid flow within the container may distribute the impregnating liquid 120 around the container, allowing it to impregnate the solid features 112.
  • the impregnating liquid may be nontoxic for occasional contact with skin because it the liquids relative inertness.
  • these materials may not be safe to eat however, but they could be suitable in many industrial applications or health and beauty applications.
  • these materials 120 can include, silicone oil, a perfluorocarbon liquid, a perfluorinated vacuum oil (such as Krytox 1506 or Fomblin 06/6), a fluorinated coolant (e.g., perfluoro-tripentyl amine sold as FC-70, manufactured by 3M), an ionic liquid, a fluorinated ionic liquid that is immiscible with water, a silicone oil comprising polydimethylsiloxane (PDMS), a silicone oil (e.g., fluorinated), fluorosilicone oil, a liquid metal, a synthetic oil, mineral oil, a vegetable oil, halocarbon oil, an electro-rheological fluid, a magneto-rheoiogical fluid
  • nontoxic liquids can be used: oleic acid, linoleic acid, triacetin, ethyl linoieate, glycerol, tributryri, tripropionin, dimethicone, peril orononyl di harmonyone, silicone fluids, amyl phthalate, any other nontoxic liquid and any combination thereof.
  • the ratio of the solid features 112 (e.g., particles) to the impregnating liquid 120 can be configured to minimize the occurrence of portions of the solid features 1 12 protruding above the liquid- product interface.
  • the solid features 1 12 make up a percentage of a surface area of the surface 110, with respect to the impregnating liquid, of less than about 15%, or less than about 5%.
  • the percentage of a surface area of the surface 110 comprising the solid features 112 can be less than about 50%, about 45%, about 40%, about 35%, about 30%, about 25%, about 20%, about 15%, about 10%), about 5%), or less than about 2%. In some embodiments, the percentage of a surface area of the surface 110 comprising the solid features 112 can be in the range of about 5% to about 50%>, about 10%> to about 30%, or about 15% to about 20%>, inclusive of ail ranges therebetween.
  • the ratio of the solid features 112 to the impregnating liquid 120 can be less than about 0.5, about 0.45, about 0.4, about 0.35, about 0.3, about 0.25, about 0.2, about 0.15, about 0.1, about 0.05, or less than about 0.02. In some embodiments, the ratio of the solid features 112 to the impregnating liquid 120 can be in the range of about 0.05 to about 0.5, about 0.1 to about 0.3, or about 0.15 to about 0.2, inclusive of all ranges therebetween. In some embodiments, a low ratio can be achieved using surface textures that are substantially pointed. By contrast, surface textures that are flat may result in higher ratios, with too much solid material being exposed at the surface.
  • the film dry weight is between about 5 x 1G "5 g/cm 2 and about 10 x 10° g/cni 2 , between about 0.1 x 10 " 5 g/cm and about 5 x 10 ""' g/cm 2 , between about 10 x 10 " 5 g/cm * and about 100 x 10 " 5 g/cm 2 , or between about 0.1 x 10° g/cm 2 and about 100 x 10° g/cm 2 , and the composition of the liquid-impregnated surface is between 3% and 5% solids, between 5% and 10%, between 10%, and 20%, between 20% and 50%, or between 50% and 70%.
  • the surface 110 may be characterized by its "complexity,” defined as being equal to (r-1) x 100%o where r is the Wenzel roughness.
  • the complexity of the surface may be at least 20% (e.g., about 23%), at least 25%, at least 45%, at least 75%, at least 100%, at least 150%, or at least 200%,.
  • a liquid-impregnated surface that is in contact with, a product defines four distinct phases (or 3 distinct phases in a close environment such as a pipe, where there is no vapor phase): an impregnating liquid, a surrounding gas (e.g., air), the product and a textured surface.
  • the interactions between the different phases determine the morphology of the contact line (i.e., the contact line that defines the contact angle of a contact liquid droplet with respect to the liquid-impregnated surface).
  • the contact line morphology substantially impacts droplet pinning and mobility of a "contact liquid" on the surface.
  • Other factors include, for example, properties of the contact liquid that affect how those materials (e.g., of water and/or product) are shed (whether they roll or slip), and what their shedding velocities are.
  • a textured surface 210 includes square microposts etched in silicon using standard photolithography processes. A photomask with square windows was used, and the pattern was transferred to photoresist using UV light exposure. Next, reactive ion etching with inductively-coupled plasma was used to etch the exposed areas to form microposts 212, such that microposts 212 are separated by interstitial region 214. Each micropost 212 had a square geometry with width "a" of about 10 urn, height h of about 10 ⁇ , and varying edge-to-edge spacing h of about 5, 10, 25, or 50 um. As shown in FIG. 4, a second level of roughness was produced on microposts 212 by creating nanograss 216.
  • micropost 212 surfaces were cleaned in Piranha solution (a mixture of sulfuric acid and hydrogen peroxide) etched in alternating flow of sulfur hexafluoride (SF 6 ) and oxygen (Q?) gases for 10 minutes, with an inductively-coupled plasma.
  • Piranha solution a mixture of sulfuric acid and hydrogen peroxide
  • SF 6 sulfur hexafluoride
  • Q oxygen
  • the samples were again cleaned in a Piranha solution and treated with a low-energy silane (octadecyltrichiorosilane (OTS)) by solution deposition.
  • OTS octadecyltrichiorosilane
  • the textured surface 210 was impregnated with the impregnating liquid 220, in this case "15 Mini "” (l ⁇ butyi ⁇ 3 ⁇ methylimidazolium bis(trifluoromethylsulfonyl) imide) (other examples of impregnating liquid may include silicone oil and DI water), by slowly dipping the textured surface (i.e., "dip-coating") into a reservoir of the lubricant.
  • the impregnating liquid 220 in this case "15 Mini "” (l ⁇ butyi ⁇ 3 ⁇ methylimidazolium bis(trifluoromethylsulfonyl) imide)
  • other examples of impregnating liquid may include silicone oil and DI water
  • ⁇ 0 the dynamic viscosity
  • ⁇ ⁇ the surface tension of the impregnating liquid 220.
  • the impregnating liquid 220 film will not spontaneously spread into the textured surface 210, as can be seen for BMIm in FIG. 5.
  • FIG. 6 shows a higher-magnification view of the region of the textured surface indicated by the arrow A in FIG. 5. Visible in FIG.
  • the impregnating film 6 are a portion of the nanotextured top surface 616 of a micropost, and a portion of the impregnating fluid 620.
  • the textured surface 210 is not coated with OTS, 0 OS ( W) > 9 C for impregnating liquids 220 as well as all b.
  • water droplets were expected to displace the hydrophobic liquid 220 and get impaled by the microposts 212 leading to significant pinning, and such behavior was confirmed, as the droplets did not roll-off of these textured surfaces.
  • the impregnating liquid 220 for example, oil may spread over and "cioak" the contact liquid, for example, a water droplet, as shown in FIG. 7A.
  • Cloaking can cause the progressive loss of the impregnating liquid 220 through entrainment in the water (or other composition) droplets as they are shed from the surface.
  • the criterion for cloaking is given by the spreading coefficient, S OW ( a ) ⁇ y wa - )>wo - Joa, where ⁇ is the interfaeiai tension between the two phases designated by subscripts w, o, and a.
  • Silicone oil OTS-treated silicon 0 0 2.0 ⁇ 5 0
  • DI water OTS-treated silicon 1 12.5 ⁇ : 0.6 95.8 ⁇ 0.5 NA NA
  • Table 3 shows surfac e and interfaeiai tension measurements and resulting spreading coefficients S OW M ::::: wa - fow " ⁇ oc , of 9.34, 96.4, and 970 cP for Dow Corning PMX
  • FIG 7C shows an 8 ⁇ water droplet placed on the silicone oil impregnated textured surface 210.
  • the droplet forms a large apparent contact angle (-100 degrees), but very close to the solid surface (red arrows in FIG. 7c) its profile changes from convex to concave.
  • a fluorescent dye was added to the silicone oil and imaged under UV light, it was observed that the point of inflection (i.e., the profi le change noted above) corresponded to the height to which an annular ridge of silicone oil was pulled up in order to satisfy a vertical force balance of the interfacial tensions at the inflection point (FIG. 7E). Although the oil was expected to have spread over the entire droplet (Fig.
  • This condition was found to be true for silicone oil, implying that the tops of the microposts 212 should be covered by a stable thin oil film.
  • This film was observed experimental ly using laser confocal fluorescence microscopy (LCFM); the micropost 212 tops appear bright due to the presence of a fluorescent dye that was dissolved in the oil (FIG, 7G).
  • Environmental SEM images of the surface (FIG. 71) show the oil-filled texture, and confirm that this film is less than a few microns thick, consistent with prior estimates for completely- wetting films.
  • thermodynamic framework is outlined that can predict which of the above- noted 12 states will be stable for a given contact liquid droplet, impregnating liquid 220, and textured surface 210 substrate material.
  • There are three possible configurations to consider for the interface "outside" of the droplet i.e., not directly adjacent to or beneath the droplet, but rather spaced from the droplet, e.g., horizontally
  • three possible configurations to consider for the interface "underneath the droplet” e.g., in a water environment.
  • These configurations are shown in FIG. 8, along with the total interface energy of each configuration.
  • the configurations possible outside the droplet are A I (not impregnated, i.e.
  • the stable configuration will be the one that has the lowest total interface energy.
  • a textured surface for example, textured surface 210
  • AL A2 the lowest energy
  • A3 the lowest total interface energy
  • ⁇ is the fraction of the projected area of the surface that is occupied by the solid and r is the ratio of total surface area to the projected area of the solid.
  • ⁇ is the fraction of the projected area of the surface that is occupied by the solid and r is the ratio of total surface area to the projected area of the solid.
  • the interface beneath the droplet upon contact with water, the interface beneath the droplet will attain one of the three different states - ⁇ Wl, W2, or W3 (FIG. 8) - depending on which has the lowest energy.
  • the stability requirements take a form similar to Eqs (3), (4), and (6), with y oa , y M , 0 m(a ), S OS ( a) , replaced with y ow , y sw , ⁇ 0 ,, Sasfw) respectively.
  • FIG. 9 Combining the above criteria along with the criterion for cloaking of the water droplet by the oil film described herein, the various possible states can be organized in a regime map, as shown in FIG. 9.
  • the cloaking criterion is represented by the upper two schematic drawings. For each of these cases, six different configurations are possible depending on how the oil interacts with the surface texture in the presence of air (vertical axes in FIG. 9) and water (horizontal axes in FIG. 9).
  • the vertical and horizontal axes are the normalized spreading coefficients S OS (a) /yoa and S OS ( W ) /y ow respectively. Considering first the vertical axis of FIG.
  • FIG. 9 shows that there can be up to three different contact lines, two of which can get pinned on the texture.
  • the degree of pinning determines the roll-off angle a* the angle of inclination at which a droplet placed on the textured solid begins to move.
  • Droplets that completely displace the oil are not expected to roll off the surface. These states are achieved when > @c as is the case for both BMI-Im and silicone oil impregnated surfaces when the silicon substrates are not treated with OTS (see Table 1). As expected, droplets did not roll off of these surfaces.
  • Droplets in states with emergent post tops are expected to have reduced mobility that is strongly texture dependent, whereas those in states with encapsulated posts outside and beneath the droplet (the A3- W3 states in FIG. 8) are expected to exhibit no pinning and consequently infinitesima!ly small roll-off angles.
  • FIG. 10A shows measurements of roll-off angles for 5 ⁇ L water droplets on silicone oil impregnated and BMIm impregnated textures, with varying post spacing b.
  • the same textures without an impregnating liquid no impregnating liquid, which is the conventional super impregnating case
  • the silicone oil encapsulated surfaces have extremely low rol l-off angles regardless of the post spacing b and oil viscosity, showing that contact line pinning was negligible, as predicted for a liquid droplet in an A3-W3 state with no contact lines on the textured substrate.
  • BMIm impregnated textures showed much higher roll-off angles, which increased as the spacing decreased - a trend that is similar to Cassie droplets on super impregnating surfaces. This observation shows that pinning was significant in this case, and occurs on the emergent post tops, (as shown in FIG. 10B). Pinning on BMIm impregnated textures was significantly reduced by adding a second smaller length scale texture (i.e. nanograss) to the posts, so that BMIm impregnated the texture even on the post tops, thereby substantially reducing ⁇ (FIG. I OC).
  • a second smaller length scale texture i.e. nanograss
  • the roll-off angle decreased from over 30 degrees (for BMIm impregnated posts without nanotexture) to only about 2 degrees (for BMIm impregnated posts with nanotexture). Note that the reduction in the emergent area fraction ⁇ is not due to the absolute size of the texture features, since the oil-water and oil-air interfaces intersect surface features at contact angles 9 OS (, v) and ⁇ 0 »( ⁇ ), and ⁇ depends on these contact angles and feature geometry.
  • Pinning results from contact angle hysteresis of up to two contact lines: an oil-air-solid contact line with a pinning force per unit length given by y oa ⁇ c s6 t ecosta) ⁇ cos&adKos(a)), and an oil-water-solid contact line with a pinning force per unit length given by y ow (cos0 reCiOS ( W ) - cos6 v . 05(3 ⁇ 4 ).
  • the length of the contact line over which pinning occurs is expected to scale as 3 ⁇ 4 ⁇ ⁇ " ⁇ where ⁇ 1, is the fraction of the droplet perimeter ( ⁇ 3 ⁇ 4) making contact with the emergent features of the textured substrate.
  • a force balance tangential to the surface gives: p gsm ⁇ R b / ⁇ icos 0 m consider (w) - cos ⁇ ⁇ ⁇ w .)
  • V increases with a and ⁇ because both increase the gravitational force acting on the droplet.
  • V decreases with ⁇ . 0 and ⁇ because both increase the resistance to droplet motion.
  • Eq. (13) is similar to that for viscous droplets rolling on completely non-wetting surfaces though additional terms are present due to the presence of the impregnated oil.
  • the three terms on the right side of Eq. (13) represent the rate of viscous dissipation within the droplet (i), in the oil film beneath the droplet and in the wetting ridge near the three-phase contact line (III).
  • the ⁇ can be less than about 0.30, about 0,25, about 0.20, about 0.15, about 0.10, about 0.05, about 0.01, or less than about 0.005. In some embodiments, ⁇ can be greater than about 0.001 , about 0.005, about 0.01 , about 0.05, about 0.10, about 0.15, or greater than about 0.20. In some embodiments, ⁇ can be in the range of about 0 to about 0.25. In some embodiments, ⁇ can be in the range of about 0 to about 0.01. In some embodiments, ⁇ can be in the range of about 0.001 to about 0.25. in some embodiments, ⁇ can be in the range of about 0.001 to about 0.10.
  • a liquid-impregnated surface for example the liquid- impregnated surface 100, 200, or any of the liquid- impregnated surfaces described herein can be configured such that cloaking by the impregnating liquid can either be eliminated or induced.
  • impregnating liquids that have S ow ( a) less than 0 will not cloak, resulting in no loss of impregnating liquids, whereas impregnating liquids that have S 0W( a) greater tha 0 will cloak a product P in contact with the liquid- impregnated surface (e.g., food products, drags, health and beauty products, water, bacterial colonies, etc.) and this may be exploited to prevent corrosion, fouling, etc.
  • cloaking can be used for preventing vapor-liquid transformation (e.g., water vapor, metallic vapor, etc.).
  • cloaking can be used for inhibiting liquid-solid formation (e.g., ice, metal, etc.). in some embodiments, cloaking can be used to make reservoirs for carrying the materials, such that independent cloaked materials can be controlled and directed by external means (like electric or magnetic fields).
  • liquid-solid formation e.g., ice, metal, etc.
  • cloaking can be used to make reservoirs for carrying the materials, such that independent cloaked materials can be controlled and directed by external means (like electric or magnetic fields).
  • cloaking can be desirable and can be used as a means for preventing environmental contamination, like a time capsule preserving the contents of the cloaked material. Cloaking can result in encasing of the material thereby cutting its access from the environment. This can be used for transporting materials (e.g., bioassays) across a length in a way that the material is not contaminated by the environment.
  • materials e.g., bioassays
  • the amount of cloaking can be controlled by various lubricant properties such as viscosity, surface tension of the impregnating liquid. Additionally or alternatively, the de-wetting of the cloaked material can also be controlled to release the material, for example a system in which a product is disposed on the liquid- impregnated surface at one end, and upon reaching the other end is exposed to an environment that causes the product to uncloak.
  • the impregnating liquid can be selected to have a S ow ( a) less than 0.
  • liquid-impregnated surfaces described herein can have advantageous droplet roll-off properties that minimize the accumulation of the contacting liquid on the surfaces.
  • a roll-off angle "a" of the liquid- impregnated surface in some embodiments can be less than about 50°, less than about 40°, less than about 30°, less than about 25°, or less than about 20°.
  • mayonnaise which is a Bingham plastic, has a viscosity that approaches infinity at low shear rates (it is non-Newtonian), and therefore behaves like a solid as long as shear stress within it remains below a critical value.
  • honey which is Newtonian
  • the flow is much slower.
  • h and R are of the same order of magnitude, and is the same.
  • ⁇ ⁇ / ⁇ 2 can he greater than about 1, about 0.5, or about 0.1.
  • the impregnating liquid includes an additive to prevent or reduce evaporation of the impregnating liquid, for example a surfactant.
  • the surfactants can include, but are not limited to, docosenoic acid, trans- 13 -docosenoic acid, cis- 13 -docosenoic acid, nonyiphenoxy tri(ethyleneoxy) ethanoi, methyl 12-hydroxyoctadecanate, 1- Tetracosanol, fluoroehemical "L-1006", and any combination thereof.
  • the additives can include Ci 6 H 3 COOH, C 17 H 33 COOH, CjgifeCOGH, ( VJ h :( ()()! I. Ci 4 H 29 OH, CieHssOH, dsH. OH, C 2 oH 4 i01:I, C 22 H 45 OH:, ⁇ V) ' OOCI h.
  • any of the liquid- impregnated surfaces described herein can include non-toxic materials, for example impregnating liquid and/or solid (e.g., solid particles used to form solid features such as, for example, wax), that are non-toxic to humans and/or animals.
  • Non-toxic liquid-impregnated surfaces can therefore be safely disposed on surfaces, for example the interior surface(s) of containers that are configured to house products formulated for human use or consumption.
  • Such products can include, for example food products, drugs (e.g., FDA approved drugs), or health and beauty products.
  • the solid features (e.g., solid particles) and/or the impregnating liquid can be removed or depleted from the surface due to friction and abrasion due to product sliding over the liquid-impregnated surface.
  • the impregnating liquid may be particularly prone to being depleted from the surface by entrainment within the product or dissolution into the product.
  • the concentration of the depleted impregnating liquid entrained in the product can be in the range of about 5 ppm to about 500 ppm, which is not negligible. Therefore, there is a need for liquid impregnating surfaces that include impregnating liquid and/or solids (e.g., solid particles that form the solid features) that are non-toxic and safe for human use or consumption.
  • any solvents used in the processing of any components of the liquid-impregnated surface may remain in the liquid-impregnated surface in some concentration, and thus the solvents can also be chosen to be non-toxic.
  • solvents that are nontoxic in residual quantities include ethyl acetate, ethanol (e.g., 200 proof, 140 proof), water, or any other non-toxic solvent.
  • the solvent may comprise ethyl acetate and/or heptane.
  • the non-toxicity requirements can vary depending upon the intended use of the product in contact with the liquid-impregnated surface.
  • liquid-impregnated surfaces configured to be used with food products or products classified as dmgs would be required to have a much higher level of non-toxicity when compared with products meant to contact only the oral mucosa (e.g., toothpaste, mouth wash, etc.), or applied topically such as, for example, health and beauty products (e.g., hair gel, shampoo, lotion, cosmetics, etc.).
  • the non-toxic liquid-impregnated surface can be disposed on a substrate, for the example, the interior wall of a container configured to house a food product or an ingredient of a food product for consumption by a human or an animal.
  • the substrate can be any surface, for example a surface of a food processing equipment that makes contact with food or food ingredients.
  • the food product or food ingredient can include, for example, a sticky, highly viscous, and/or non-Newtonian food product.
  • Such food products can include, for example, candy, chocolate syrup, mash, yeast mash, beer mash, taffy, food oil, fish oil, marshmaliow, dough, batter, baked goods, chewing gum, bubble gum, butter, peanut butter, jelly, jam, dough, gum, cheese, cream, cream cheese, mustard, yogurt, sour cream, curry, sauce, ajvar, currywurst sauce, salsa iizano, chutney, pebre, fish sauce, tzatziki, sriracha sauce, vegemite, cursehuni, HP sauce/brown sauce, harissa, kochujang, hoisin sauce, kim chi, cholula hot sauce, tartar sauce, tahini, hummus, shichimi, ketchup, mustard, pasta sauce, Alfredo sauce, spaghetti sauce, icing, dessert toppings, or whipped cream, liquid egg, ice cream, animal food, any other food product or combination thereof.
  • the components of the non-toxic liquid-impregnated surfaces can include materials that are non-toxic when consumed orally by a human or an animal.
  • the liquid-impregnated surface can include materials that are a U.S. Food and Drug Administration (FDA) approved direct or indirect food additive, an FDA approved food contact substance, satisfy FDA regulatory requirements to be used as a food additive or food contact substance, and/or is an FDA GRAS material. Examples of such materials can be found within the FDA Code of Federal Regulations Title 21 , located at ii http:/7wwwMccessdaM lia.go ' Wscrip the entire contents of which are hereby incorporated by reference herein.
  • FDA U.S. Food and Drug Administration
  • the components of the non-toxic liquid-impregnated surface can exist as a component of the food product disposed within the container.
  • the components of the non-toxic liquid-impregnated surface can include a dietary supplement or ingredient of a dietary supplement.
  • the components of the non-toxic liquid-impregnated surface can also include an FDA approved food additive or color additive.
  • the non-toxic liquid impregnating surface can include materials that exist naturally in, or are derived from plants and animals.
  • the nontoxic liquid-impregnated surface for use with food products includes solids or impregnating liquid that are flavorless or have a high flavor threshold of below 500 pprn, are odorless or have high odor threshold, and/or are substantially transparent.
  • the non-toxic liquid-impregnated surface for use with food products includes solids or impregnating liquid that are tasteless and/or immiscible with an adjacent phase.
  • the non-toxic liquid-impregnated surface can be disposed on a substrate, for the example, the interior side wall of a container configured to house a drug or products classified as a drug, for example, an FDA approved dr g for consumption by a human or an animal.
  • the drug can be in the form of a liquid, a cream, an ointment, a lotion, an eye drop, an oral drug, an intravenous drug, an intramuscular drug, a suspension, a colloid, or any other form and can include any drug included within the FDA's database of approved drugs.
  • the materials included in the non-toxic liquid- impregnated surface can include an FDA approved drag ingredient, for example any ingredient included in the FDA's database of approved drugs, '%ttp://www ccessdata.fda.gov/scripts/cder/dmgsatfda/index fii3 ⁇ 4" the entire contents of which are hereby incorporated herein by reference.
  • the non-toxic liquid-impregnated surface can include materials that satisfy FDA requirements to be used in drags or are listed within the FDA's National Drag Discovery Code Directory, ' i http://ww r w.accessdata.fda,gov/scripts/cder/ndc/default.cfm'', the entire contents of which are hereby incorporated herein by reference.
  • the materials can include inactive drug ingredient of an approved drug product as listed within FDA's database, "http://www.accessdata.fda.gov/scripts/cder/ndc/defaultxrrn", the entire contents of which are hereby incorporated herein by reference.
  • the materials can include any materials that satisfy the requirement of materials that can be used in liquid-impregnated surfaces configured to be used with food products, and or include a dietary supplement or ingredient of a dietary supplement.
  • the non-toxic liquid-impregnated surface can be disposed on a substrate, for the example, the interior side wall of a container configured to house a health and beauty product which is also classified as a drug.
  • Examples of such product can include, but are not limited to toothpaste, sun screens, anti-perspirants, anti-dandruff shampoos, anti-dandruff conditioners, or anti-bacterial cleansers
  • the health and beauty product for example, toothpaste can include an impregnating liquid and/or a solid which is FDA approved and satisfies FDA drug requirements as are listed within the FDA's National Drug Discovery Code Directory and can also include FDA approved health and beauty ingredient, that satisify FDA requirements to be used in health and beauty products, satisfies FDA regulatory laws mcluded in the Federal Food, Drag and Cosmetic Act (FD&C Act), or the Fair Packaging and Labeling Act (FPLA).
  • FD&C Act Federal Food, Drag and Cosmetic Act
  • FPLA Fair Packaging and Labeling Act
  • the non-toxic liquid-impregnated surface can be disposed on a substrate, for the example, the interior side wall of a container configured to house a health and beauty product, which does not include a compound classified by FDA as a drug compound or an active ingredient of a drug.
  • a health and beauty product which does not include a compound classified by FDA as a drug compound or an active ingredient of a drug.
  • Such products can include product configured to contact the oral mucosa, for example non-fluoride toothpaste, some mouth washes, mouth creams, denture fixing compounds, or any other oral hygiene product.
  • the health and beauty product can include a products configured for topical application, for example cosmetics, lotions, shampoo, conditioner, moisturizers, face washes, hair-gels, medical fluids (e.g., anti-bacterial ointments or creams), any other health or beauty product, and or combination thereof.
  • the non-toxic liquid impregnated coating can include, for example, a material that is an FDA approved health and beauty ingredient, or that satisfies FDA requirements to be used in health and beauty products, FDA regulatory laws included in the Federal Food, Drug and Cosmetic Act (FD&C Act), and/or the Fair Packaging and Labeling Act (FPLA).
  • the solids and or impregnating liquid included in the non-toxic liquid-impregnated surface can include a flavor or a fragrance.
  • the materials included in any of the non-toxic liquid- impregnated surfaces described herein can be flavorless or have high flavor thresholds below 500 ppm, and can be odorless or have a high odor threshold.
  • the materials included in any of the non-toxic liquid impregnating surfaces described herein can be substantially transparent.
  • the solid and the impregnating liquid can be selected so that they have substantially the same or similar indices of refraction. By matching their indices of refraction, they may be optically matched to reduce light scattering and improve light transmission.
  • the materials included in the liquid-impregnated surfaces are organic or are derived from organically grown products.
  • the liquid surface film includes a liquid having a melting point that is higher than the temperature at which the container bearing said liquid surface film would typically be stored, shipped, transported, etc.
  • the liquid may be frozen during certain such periods.
  • the liquid surface film dissolves much more slowly (e.g., in the presence of an adjacent product), and to a lesser extent, thereby enhancing the lifetime of the liquid surface film during storage.
  • the liquid surface film Upon thawing, the liquid surface film regains the performance characteristics that it had prior to freezing (i.e., its "slippery" properties).
  • This ability to freeze the liquid component of the liquid surface film may be desirable, for example, during periods of time when the liquid surface film has been applied to a container but the container does not yet contain a product, or when a product within a container coated with the liquid surface film does not yet need to be dispensed (e.g., during shipment or storage).
  • the materials included in any of the non-toxic liquid- impregnated surfaces described herein can be recyclable.
  • the solid or impregnating liquid can include materials that wash away during standard container (e.g., glass bottle, plastic bottle, etc.) recycling process.
  • the liquid-impregnated surface can be configured to pass standard recycling tests provided by the Association for Postconsumer Plastic Recyclers (e.g., may be adequately cleaned using the typical wash used in PET bottle recycling).
  • the liquid-impregnated surface can be configured to dissolve in a caustic wash, for example a solution of Triton X 100 or NaOH at high temperature, an acid wash, a solvent wash, or any other dissolving solution,
  • the impregnating liquid included in the non-toxic liquid- impregnated surface can include one or more additives.
  • the additive can be configured, for example, to reduce the viscosity, vapor pressure, or solubility of the impregnating liquid.
  • the additive can be configured to increase the chemical stability of the liquid-impregnated surface.
  • the additive can be an antioxidant configured to inhibit oxidation of the liquid-impregnated surface.
  • the additive can be added to reduce or increase the freezing point of the liquid.
  • the additive can be configured to reduce the diffusivity of oxygen or C0 2 through the liquid- impregnated surface or enable the liquid-impregnated surface to absorb more ultra violet (UV) light, for example protect the product (e.g., any of the products described herein), disposed within a container on which the non-toxic liquid-impregnated surface is disposed.
  • the additive can be configured to provide an intentional odor, for example a fragrance (e.g., smell of flowers, fruits, plants, freshness, scents, etc.).
  • the additive can be configured to provide color to the liquid-impregnated surface and can include, for example a dye, or an FDA approved color additive.
  • the non-toxic liquid-impregnated surface includes an additive that can be released into the product, for example, a flavor or a preservative.
  • the materials included in any of the non-toxic liquid- impregnated surfaces described herein can be organic or derived from organically grown products.
  • the impregnating liquids can include organic liquids that are often or sometimes non-toxic.
  • Such non-toxic organic liquids can, for example, include materials that fall within the following classes: lipids, vegetable oils (e.g., olive oil, light olive oil, corn oil, soybean oil, rapeseed oil, linseed oil, grapeseed oil, flaxseed oil, peanut oil, safflower oil, palm oil, coconut oil, or sunflower oil), fats, fatty acids, derivatives of vegetable oils or fatty acids, esters, terpenes, monoglycerides, diglycerides, triglycerides, mixtures of triglycerides such as MCT oil (medium chain triglyceride oil), triacetin, tripropio in, alcohols, and fatty acid alcohols.
  • vegetable oils e.g., olive oil, light olive oil, corn oil, soybean oil, rapeseed oil, linseed oil, grapeseed oil, flaxseed oil, peanut oil, safflower oil, palm oil, coconut oil, or sunflower oil
  • fats
  • any of the non-toxic liquid-impregnated surfaces described herein can include organic solids, semi-solids, and/or liquids that are non-toxic and that fall within the following classes: lipids, waxes, fats, fibers, cellulose, derivatives of vegetable oils, esters (such as esters of fatty acids), terpenes, monoglycerides, diglycerides, triglycerides, alcohols, triacetin, tripropionin, citric triglycerides, propylene glycol, poly ethylene glycol, fatty acid alcohols, ketones, aldehydes, proteins, sugars, salts, minerals, vitamins, carbonate, ceramic materials, alkanes, alkenes, alkynes, acyl halides, carbonates, carboxylates, carboxylic acids, methoxies, hydroperoxides, peroxides, ethers, hemiacetais, hemiaketals, acetals, ket
  • any of the non-toxic liquid-impregnated surfaces can include inorganic materials, for example ceramics, metals, metal oxides, silica, glass, plastics, any other inorganic material or combination thereof.
  • any of the non-toxic liquid- impregnated surfaces described herein can include, for example preservatives, sweeteners, color additives, flavors, spices, flavor enhancers, fat replacers, and components of formulations used to replace fats, nutrients, emulsifiers, surfactants, bulking agents, cleansing agents, depilatories, stabilizers, emulsion stabilizers, thickeners, flavor or fragrance, an ingredient of a flavor or fragrance, binders, texturizers, humectants, pH control agents, aciduiants, leavening agents, anti-caking agents, anti-dandruff agents, anti-microbial agents, anti-perspirants, anti-seborrheic agents, astringents, bleaching agents, denaturants, depilatories, emollients, foaming agents, hair conditioning agents, hair fixing agents, hair waving agents, absorbents, anti-corrosive agents, anti-foaming agents, anti-oxidants, anti-
  • the non-toxic liquid-impregnated surface can include nontoxic materials having an average molecular weight in the range of about 100 g/mol to about 600 g/mol. which are included in the Springer Material Landolt-Bornstein database located at, 'littp!/A ⁇ v-springem aterials-Com ⁇ ocs/index-html,'' or in the MatNavi database located at "www.mits.nims.go.jp/index en. html.”
  • the liquids have boiling points greater than 150 °C, for example 250°C or below about 270TJ, such that they are not classified as volatile organic compounds (VOC's).
  • a liquid- impregnated surface can include an impregnating liquid whose density is substantially equal
  • the ratio of impregnating liquid density to product density may be in a range from 0.95: 1 to 0.95: 1.1 .
  • the density of the impregnating liquid may be about 1 g/enr.
  • the liquid can include materials safe for skin contact or one that is a ingredient in a health and beauty product.
  • materials safe for skin contact include silicone oils, fluorinated hydrocarbons, fluorinated perfluoropoiyethers, fluorinated silicones, aryl silicones, phenyl trimethicone, cyclomethicones, aryl cyclomethicor.es and hydrocarbon liquids including mineral oil, paraffin oil, C13-C14 isoparaffins, C16-C18 isoparaffms, di- and trig!ycyceride esters, tri alkyl esters of citric acid.
  • the solid material can include materials safe for skin contact or one that is a ingredient in a health and beauty product.
  • materials safe for skin contact or one that is a ingredient in a health and beauty product.
  • examples include the categories of silicones, alkyl silicone waxes, hydrocarbon waxes, polymethylsilsesquioxane partilces, silica particles wit hydrophobic treatment (for example a hydrophobic silane), silica particles with polydimethyl siloxane (PDMS) resin outer layer, polymethylsilsesquioxane partilces with polydimethyisiioxane resin outer layer, silicone prepolymer mixes with combinations of silica and PDMS particles, UV curable PDMS.
  • silicones for example a hydrophobic silane
  • PDMS polydimethyl siloxane
  • silicone prepolymer mixes with combinations of silica and PDMS particles UV curable PDMS.
  • the textured solid and the impregnating liquid prefferably have substantially similar chemistry, such that the liquid has a high affinity for the solid and preferentially wet it beneath a product.
  • the solid could be PDMS and/or a siliconyl wax, and the liquid could be a silicone oil or dimethicone.
  • These classes of materials are found to be effective combinations for coatings for many consumer products including many hair gels, conditioner, and oil in water lotions.
  • Another effective combination are waxes that are food additives used as a solid that are impregnated with a liquid having substantially similar chemistry.
  • the solid could be a triglyceride based wax and the liquid could be a triglyceride.
  • a first surface having a matrix of solid features was prepared by Procedure 1, described as follows. A mixture was made by heating about 40 mL of ethanol to a temperature of about 85 °C, slowly adding about 0.4 grams of camauba wax powder, boiling the mixture for approximate!)' 5 min, and then allowing the mixture to cool while being sonicated for about 5 min. The resulting mixture was sprayed onto a substrate with the airbrush (at an airbrush pressure of about 50 psi), and then allowed to dry at ambient temperature and humidity for about 1 min. SEM images of the resulting surface are shown in FIGS 12 and 13 (at 500X and 15,000X magnification, respectively).
  • a second surface was prepared by Procedure 2, described as follows. A mixture was made by adding about 4 grams of powdered camauba wax to about 40 mL ethanol and vigorously stirring. The resulting mixture was sprayed onto a substrate with the airbrush (at an airbrush pressure of about 50 psi) for about 2 seconds at a distance of about 4 inches from the surface, and then allowed to dry at ambient temperature and humidity for about 1 min. SEM images are shown in FIGS 14 and 15 (at 500X and 15,000X magnification, respectively).
  • a third surface was prepared by Procedure 3, described as follows. An aerosol wax was sprayed onto a substrate at a distance of about 10 inches for about 3 seconds. The spray nozzle was moved such that spray residence time was no longer than about 0.5 sec/unit area, and then the substrate was allowed to dry at ambient temperature and humidity for about 1 min. SEM images are shown in FIGS 16 and 17 (at 500X and 15,000X magnification, respectively).
  • a quantity of about 5 to about 10 ml. of ethyl oleate (sigma Aldricb) or vegetable oil was swirled around in bottles that initially had an internal surface entirely covered with wax (prepared by Procedure 3 as described above), until the bottles became transparent.
  • Such a coating time was chosen so that a cloudy (not patchy) coating formed over the whole internal surface.
  • the formed coating had a thickness in a range of about 10 microns to about 50 microns.
  • FIGS. 18 through 23 show time-lapse images of a volume of ketchup on a liquid- impregnated surface, prepared in accordance with an embodiment of the invention.
  • the spot of ketchup was able to slide along the liquid-impregnated surface due to a slight tilting (e.g., about 5 to about 10 degrees) of the surface.
  • the ketchup moved along the surface as a substantially rigid body, without leaving any ketchup residue along its path.
  • the elapsed time from FIG. 18 to FIG. 23 was about 1 second.
  • a liquid-impregnated surface which included carnauba wax mixed trichloroethylene as the solid, was impregnated with methyl laurate, which has a freezing point of 5°C.
  • One PET bottle was coated with carnauba wax impregnated with methyl laurate, and another one was coated with carnauba wax impregnated with ethyl oleate, which has a freezing point of -32°C.
  • Both PET bottles were filled with scrambled egg yolk, and showed nearly identical siipperiness at room temperature, based on the sliding speed of about 3 scrambled egg yolks at a 15° angle.

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Abstract

Les formes de réalisation de la présente invention concernent de manière générale des contenants, sur les surfaces intérieures desquels des surfaces imprégnées de liquide sont placées. Les surfaces imprégnées de liquide forment un aménagement d'éléments solides et/ou semi-solides délimitant entre eux une ou plusieurs régions interstitielles, un liquide d'imprégnation imprégnant de préférence ces régions. Les contenants peuvent être conçus pour contenir un produit destiné à la consommation humaine ou animale. Les éléments solides et/ou semi-solides et le liquide d'imprégnation délimitent collectivement une surface secondaire (p. ex. sensiblement parallèle à la surface intérieure sur laquelle les surfaces imprégnées de liquide sont placées) et peuvent comprendre des matières non toxiques. Les surfaces imprégnées d'un liquide non toxique de l'invention peuvent en particulier être conçues pour être utilisées dans des produits alimentaires, des médicaments, des produits de santé et/ou de beauté.
EP14844341.9A 2013-09-16 2014-09-16 Surfaces imprégnées d'un liquide non toxique Withdrawn EP3046755A4 (fr)

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