Invisible-fingerprint coatings and method for forming the same

Abstract

To provide an article having a coating that can provide optical transparency, mechanical durability, and invisible fingerprint properties, and a method for forming an invisible fingerprint coating.SOLUTION: A process for forming a coating on a substrate comprises the steps of: forming a non-fluorinated alkyl silane hydrolysate polymer; and applying the non-fluorinated alkyl silane hydrolysate polymer to a surface of the substrate. The formed invisible-fingerprint coating can have an initial oil angle of less than 50°.SELECTED DRAWING: Figure 11

Description

[Technical Field]

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS This application claims the benefit of U.S. Provisional Patent Application No. 62 / 812,329, filed March 1, 2019, the entire disclosure of which is incorporated herein by reference.

[0002] The present invention, in an exemplary embodiment, relates to a coating composition for coating a substrate to make fingerprints invisible or nearly invisible. [Background technology]

[0003] People naturally produce sebum (from sebaceous glands) and other oils on their faces and fingertips. People can deposit such oils on the display screen of a mobile phone (or other object), such as glass (or a screen protector, usually a polymer or plastic), glass ceramic, metal oxide, Plexiglas, or similar materials or surfaces. Often, such oils are visible and can degrade the quality of images viewed on such devices, as well as contribute to a poor aesthetic appearance of the screen (along with dirt, dust, etc.). Fingerprint-invisible ("IFP") coatings are typically oleophilic coatings that make oils invisible or nearly invisible by spreading them along the screen surface. The deposited oils can match the refractive index of the screen material, e.g., glass, resulting in light passing through and making the fingerprint appear absent. Fingerprints may still be present, but they cannot be seen (at least without closely examining the surface).

[0004] One of the more significant challenges for optically transparent substrates and coatings is mechanical abrasion, which can degrade, wear away, or reduce the thickness, transparency, or effectiveness of the coating. Abrasion occurs to a greater or lesser extent during user handling of the substrate, for example, by rubbing with a cloth to remove fingerprints or smudges, which is periodically required to restore adequate visibility, especially through transparent substrates. Degradation can also occur due to exposure to ultraviolet light, heat, cold, chemicals, salt or other corrosive substances, dirt, other abrasives, or other environmental elements, conditions, or materials.

[0005] In contrast to IFPs, "fingerprint-resistant" ("AFP") coatings are oil-repellent coatings that resist wetting. Because of their oil-repellent properties, fingerprints can be formed and then wiped off. IFP coatings function in a different manner than AFP coatings.

[0006] It is desirable to have a coating that can provide optical clarity, mechanical durability, and fingerprint invisibility. Summary of the Invention

[0007] The following presents a simplified summary in order to provide a basic understanding of some aspects of various invention embodiments. This summary is not an extensive overview of the invention. It is not intended to identify key or critical elements of the invention or to delineate the scope of the invention. The following summary merely presents some concepts of the invention in a simplified form as a prelude to the more detailed description below.

[0008] The present invention, in exemplary embodiments, relates to compositions and formulations for providing IFP coatings.

[0009] In one aspect, the present invention provides an article comprising: A substrate; a fingerprint-invisible coating laminated to the substrate; The fingerprint-invisible coating relates to an article comprising a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da.

[0010] In another aspect, the present invention provides an article comprising: A substrate; a fingerprint-invisible coating laminated to the substrate; the fingerprint-invisible coating comprises a non-fluorinated alkylsilane hydrolyzate polymer; The non-fingerprint coating relates to an article having a thickness of less than 1000 nm. In some embodiments, the thickness is greater than 0.1 nm.

[0011] In another aspect, the present invention provides a fingerprint-invisible composition comprising: a solvent; and a non-fluorinated alkylsilane hydrolysate polymer having a weight average molecular weight of less than 100,000 Da.

[0012] In another aspect, the present invention provides a method for forming a fingerprint-invisible composition, comprising: polymerizing an alkylsilane in a first solvent comprising water and an organic solvent to form a non-fluorinated alkylsilane hydrolyzate; and dissolving the non-fluorinated alkylsilane hydrolyzate in a second solvent to a concentration of at least 0.01 mg / L and less than 100 g / L. In some embodiments, the organic solvent is an alcohol.

[0013] In another aspect, the present invention provides a method for forming a fingerprint-invisible surface, comprising: On the surface of the substrate, A solvent; a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da and at least 300 Da; and depositing a formulation comprising: and curing the formulation to form the fingerprint-invisible surface.

[0014] In another aspect, the invention relates to an article, composition, or method described herein, wherein said non-fluorinated alkylsilane hydrolysate polymer comprises a functional group selected from the group consisting of hydroxy, carboxy, amino, halo, and combinations thereof.

[0015] Other features will become apparent from the following detailed description of certain exemplary embodiments when taken in conjunction with the appended claims. [Brief explanation of the drawings]

[0016] The drawings disclose the following exemplary embodiments or test results. [Figure 1] FIG. 1 shows the FTIR of Examples 13 to 16. [Figure 2] FIG. 2 shows the FTIR of Examples 18-21 and 11-chloroundecyltriethoxysilane, designated as "CLAS" in the figure. [Figure 3] FIG. 3 shows the FTIR of Examples 23-26 and 11-chloroundecyltriethoxysilane, designated as "CLAS" in the figure. [Figure 4] FIG. 4 shows the TGA of 11-chloroundecyltriethoxysilane. [Figure 5] FIG. 5 shows the TGA of weight loss versus temperature for 11-chloroundecyltriethoxysilane, shown in the figure as "CLAS," with water to ethoxy molar ratios of 1:2 (A), 1:1 (B), and 2:1 (C). [Figure 6] Figure 6 shows the weight loss versus temperature for polymerized derivatives of 11-chloroundecyltriethoxysilane, designated "CLAS" in the figure, at the following water to ethoxy molar ratios: 1:1 (A), 2:1 (B), and 3:1 (C). [Figure 7]Figure 7 shows the relationship between weight loss and temperature for a 14:1 ratio of 11-chloroundecyltriethoxysilane and 1,2-bis(triethoxysilyl)ethane with the following water to ethoxy molar ratios: 1:1 (A), 2:1 (B), and 3:1 (C). [Figure 8] Figure 8 shows the relationship between weight loss and temperature for a 14:1 ratio of 11-chloroundecyltriethoxysilane and 1,2-bis(triethoxysilyl)ethane at water to ethoxy molar ratios of 1:2 (A), 1:1 (B), 2:1 (C), and 3:1 (D). [Figure 9] Figure 9 shows the weight loss versus temperature for a 14:1 ratio of 11-chloroundecyltriethoxysilane and 1,1,2-tris(triethoxysilyl)ethane at the following water to ethoxy molar ratios: 1:1 (A), 2:1 (B), and 3:1 (C). [Figure 10] Figure 10 shows the weight loss versus temperature for derivatives of 11-chloroundecyltriethoxysilane and 1,1,2-tris(triethoxysilyl)ethane in a 14:1 ratio at the following water to ethoxy molar ratios: 1:1 (A), 2:1 (B), and 3:1 (C). [Figure 11] FIG. 11 shows GPC chromatograms of the hydrolysis products of 11-chloroundecyltriethoxysilane formed with unreacted 11-chloroundecyltriethoxysilane (A) at the following water to ethoxy molar ratios: 1:2 (B), 1:1 (C), 2:1 (D), and 3:1 (E). DETAILED DESCRIPTION OF THE INVENTION

[0017] As used in this specification and the appended claims, the singular forms "a," "an," and "the" include plural referents unless the context clearly dictates otherwise. It is further noted that the claims may be drafted to exclude any optional element. Accordingly, this statement is intended to serve as a basis for using exclusive terminology, such as "solely," "only," and the like, in connection with the recitation of claim elements or the use of a "negative" limitation.

[0018] As used herein, the terms "including," "containing," and "comprising" are used in their open, non-limiting sense. Throughout the description and claims of this specification, the word "comprise" and variations of that word, such as "comprising" and "comprises," mean "including, but not limited to," and are not intended to exclude, for example, other additives, ingredients, integers, or steps. "Exemplary" means "one example of" and is not intended to convey an indication of a preferred or ideal embodiment. "For example" or "specifically" are used for illustration purposes, not limitation.

[0019] In order to provide a more concise explanation, some of the quantitative expressions presented herein are not modified with the term "about." Regardless of whether the term "about" is explicitly used, all quantities presented herein are understood to refer to actual predetermined values ​​and to refer to approximations of such predetermined values ​​that can be reasonably inferred based on those skilled in the art, including equivalents and approximations based on experimental and / or measurement conditions for such predetermined values. Whenever a yield is presented as a percentage, such a yield refers to the mass of the entity from which the yield is obtained, relative to the maximum amount of the same entity that can be obtained under specific stoichiometric conditions. Concentrations presented as percentages refer to mass ratios unless otherwise indicated.

[0020] Unless otherwise specified, the methods and techniques of the present embodiments are generally carried out according to conventional methods well known in the art and as described in various general and more specific references cited and discussed throughout this specification. See, for example, Loudon, Organic Chemistry, Fourth Edition, New York: Oxford University Press, 2002, pp. 360-361, 1084-1085; Smith and March, March's Advanced Organic Chemistry: Reactions, Mechanisms, and Structure, Fifth Edition, Wiley-Interscience, 2001.

[0021] It is understood that certain features of the present disclosure that are described, for clarity, in the context of separate embodiments may also be provided in combination in a single embodiment. Conversely, for brevity, various features of the present disclosure that are described in the context of a single embodiment may also be provided separately or in any suitable subcombination. All combinations of embodiments relating to chemical groups represented by variables are specifically embraced by the present disclosure and are disclosed herein as if all combinations were individually and explicitly disclosed, to the extent that such combinations include compounds that are stable compounds (i.e., compounds or polymers that can be isolated and characterized). Furthermore, all subcombinations of chemical groups listed in embodiments describing such variables are also specifically embraced by the present disclosure and are disclosed herein as if each such subcombination of chemical groups were individually and explicitly disclosed herein. definition

[0022] As used herein, the term "alkyl" includes a chain of carbon atoms, optionally branched, containing 1 to 20 carbon atoms. In certain embodiments, alkyl includes C1-C 12 , C1~C 10It is further understood that alkyl groups of limited lengths, including C1-C9, C1-C8, C1-C7, C1-C6, and C1-C4, may be advantageous. Illustratively, such limited-length alkyl groups, including C1-C8, C1-C7, C1-C6, and C1-C4, etc., may be referred to as "lower alkyl." Exemplary alkyl groups include, but are not limited to, methyl, ethyl, n-propyl, isopropyl, n-butyl, isobutyl, sec-butyl, tert-butyl, pentyl, 2-pentyl, 3-pentyl, neopentyl, hexyl, heptyl, octyl, etc. Alkyl can be substituted or unsubstituted. Typical substituents include cycloalkyl, aryl, heteroalicyclic, alkoxy, halo, carbonyl, oxo, (═O), C-carboxy, O-carboxy, nitro, and amino, or those described in the various embodiments provided herein. It is understood that "alkyl" can be combined with other groups, such as those provided above, to form functionalized alkyls. Examples include the C1-C6 alkyls described herein. 10 The combination of an "alkyl" group, such as an alkyl group, and an "aryl" group is "C1-C 10 These groups may be referred to as "alkylaryl" groups.

[0023] As used herein, the term "alkenyl" includes a chain of carbon atoms, optionally branched, containing from 2 to 20 carbon atoms and also containing at least one carbon-carbon double bond (i.e., C=C). In certain embodiments, alkenyl includes C2-C 12 It is understood that the alkenyl group is advantageously limited in length, including C2-C9, C2-C8, C2-C7, C2-C6, and C2-C4. The alkenyl can be unsubstituted or substituted as described for alkyl or as described in the various embodiments provided herein. The at least one carbon-carbon double bond can be internal or terminal. Exemplary alkenyl groups include, but are not limited to, ethenyl, 1-propenyl, 2-propenyl, 1-, 2-, or 3-butenyl, and the like.

[0024] As used herein, the term "alkynyl" includes a chain of carbon atoms, optionally branched, containing 2 to 20 carbon atoms and also containing at least one carbon-carbon triple bond (i.e., C≡C). In certain embodiments, alkynyl includes C2-C 12 It is understood that the alkynyl group may be of any advantageously limited length, including C2-C9, C2-C8, C2-C7, C2-C6, and C2-C4. The alkynyl group may be unsubstituted or substituted as described for alkyl or as described in the various embodiments provided herein. The at least one carbon-carbon triple bond may be internal or terminal. Exemplary alkynyl groups include, but are not limited to, ethynyl, 1-propynyl, 2-propynyl, 1-, 2-, or 3-butynyl, and the like.

[0025] As used herein, the term "aryl" refers to an all-carbon monocyclic or fused-ring polycyclic group of 6 to 12 carbon atoms having a fully conjugated pi-electron system. In certain embodiments, aryl is a C6-C 10 It is understood that it may be advantageous to have a limited size such as aryl. Exemplary aryl groups include, but are not limited to, phenyl, naphthylenyl, and anthracenyl. The aryl group may be unsubstituted or substituted as described for alkyl or as described in the various embodiments provided herein.

[0026] As used herein, the term "cycloalkyl" refers to a 3- to 15-membered all-carbon monocyclic ring, including an all-carbon 5-membered / 6-membered or 6-membered / 6-membered fused bicyclic ring, or polycyclic fused ring (a "fused" ring system means that each ring in the system shares adjacent pairs of carbon atoms with each other ring in the system) group, or a carbocycle fused to another group, such as a heterocycle, such as a 5- or 6-membered cycloalkyl ring fused to a 5- to 7-membered heterocycle, wherein one or more rings may contain one or more double bonds, but the cycloalkyl does not contain a fully conjugated pi-electron system. In certain embodiments, cycloalkyl refers to a carbocycle fused to a C3-C6 13 It is understood that cycloalkyl may be advantageously of limited size, such as C3-C9, C3-C6, and C4-C6. Cycloalkyl can be unsubstituted or substituted as described for alkyl or as described in the various embodiments provided herein. Exemplary cycloalkyl groups include, but are not limited to, cyclopropyl, cyclobutyl, cyclopentyl, cyclopentenyl, cyclopentadienyl, cyclohexyl, cyclohexenyl, cycloheptyl, and the like. Illustrative examples of cycloalkyl groups shown in graphic depictions include the following entities in the form of appropriately bonded moieties:

[0027] [ka] is included.

[0028] As used herein, "halo" or "halogen" refers to chlorine, bromine, or iodine, excluding fluorine.

[0029] The term "oxo" refers to a carbonyl oxygen. For example, cyclopentyl substituted with oxo is cyclopentanone.

[0030] As used herein, "hydroxy" or "hydroxyl" refers to an --OH group.

[0031] As used herein, "alkoxy" refers to both an -O-(alkyl) or an -O-(unsubstituted cycloalkyl) group. Representative examples include, but are not limited to, methoxy, ethoxy, propoxy, butoxy, cyclopropyloxy, cyclobutyloxy, cyclopentyloxy, cyclohexyloxy, and the like.

[0032] As used herein, "oximo" refers to an oxime. For example, oximo includes, but is not limited to, the group -ON=C(R1)(R2), where R1 and R2 are any suitable substituents.

[0033] As used herein, "bond" refers to a covalent bond.

[0034] The term "substituted" means that the specified group or moiety has one or more substituents. The term "unsubstituted" means that the specified group has no substituents. When the term "substituted" is used to describe a structural system, it means that substitution occurs at any valence-allowed position on the system. In some embodiments, "substituted" means that the specified group or moiety has one, two, or three substituents. In other embodiments, "substituted" means that the specified group or moiety has one or two substituents. In yet other embodiments, "substituted" means that the specified group or moiety has one substituent.

[0035] As used herein, "optionally" or "optionally" means that the subsequently described event or circumstance may occur, but need not occur, and the description encompasses both cases where the event or circumstance occurs and cases where it does not occur. For example, "C1-C 20 "Each hydrogen atom of the alkyl is optionally substituted with a halogen" means that by substituting a hydrogen atom with each halogen, C1 to C 20 The description means that halogens may be present in any of the alkyls, but do not have to be present.20 The situation where the alkyl is not substituted with halogen is included.

[0036] As used herein, "independently" means that the event or circumstance described thereafter is to be read on its own in comparison with other similar events or circumstances. For example, in a situation where several equivalent hydrogen groups are optionally replaced by another group described in the situation, the use of "independently and optionally" means that each instance of a hydrogen atom on the group can be replaced by another group, and the groups replacing each of the hydrogen atoms can be the same or different. Or, for example, when there are multiple groups, all of which can be selected from a set of possibilities, the use of "independently" means that each of the groups can be selected from a set of possibilities separate from the other groups, and the groups selected in that situation can be the same or different.

[0037] A fingerprint-invisible article, sometimes referred to as an IFP article, according to the present disclosure includes a substrate surface coated with a fingerprint-invisible coating, sometimes referred to as an IFP coating. Illustratively, the fingerprint-invisible coating can be formed on the surface by a method including applying a fingerprint-invisible coating formulation to the substrate surface. In some embodiments, the fingerprint-invisible coating formulation includes a hydrolyzate of an alkylsilane, such as a non-fluorinated alkylsilane. In some embodiments, the formulation further includes an alkylsiloxane. In some embodiments, the formulation is applied to the substrate surface using spraying, chemical vapor deposition (CVD), or physical vapor deposition (PVD). Illustratively, it may be desirable to minimize the presence of acids, which can lead to cloudiness of the surface. In some embodiments, the formulation is substantially acid-free.

[0038] In exemplary embodiments, the substrate may be a glass screen, such as those used in electronic displays, including, but not limited to, cell phone screens, computer monitors, television screens, touchscreens, home appliances, head-up displays, eyewear (e.g., eyeglasses and sunglasses), masks (e.g., welding masks), interior wall paint, and the like. In exemplary embodiments, the substrate may also be used in the appliance and cosmetic finish fields, such as decorative panels for appliances, particularly household appliances (refrigerator doors, oven doors, display cases, and the like). The substrate may be made of glass (or screen protectors, typically polymers or plastics), glass ceramic, metal oxide, Plexiglas, or other materials. In some embodiments, the substrate comprises glass, glass ceramic, metal oxide, or plastic. In some embodiments, the surface is soda-lime glass or AlSiO glass. Additional substrates include car interior components or household items such as casings, blinds, decorative frames, and handles; plumbing fixtures such as sink plugs, faucets, and mixers; and general office equipment. Particularly suitable are glass and metal surfaces with low roughness (0.3-1.0 μm) and metallized surfaces.

[0039] In this disclosure, the term "invisible" should be understood to include invisible, invisible, barely visible, or unnoticeable (e.g., not visible without close inspection of the surface). It should also be understood that "invisibility" depends, to some extent, on light refraction and the viewing direction of the surface. From certain angles, fingerprints may be invisible, while from other angles they may be discernible. The term "wettability" refers to the propensity of polar or non-polar liquids to adhere to a substrate and form undesirable films, as well as the tendency of the substrate to attract all kinds of dust, dirt, fingerprints, insects, etc. Fingerprint resistance (AFP) enhances water and oil repellency, while IFP selectively alters the surface tension of different fluids, such as water and oil, making the surface both hydrophobic and oleophilic at the same time.

[0040] One approach to achieving a fingerprint-invisible coating involves optimizing the water and oil contact angles so that the resulting liquid spreads across the surface and matches the refractive index of the liquid on the surface with the glass substrate. In such a case, light passes through the fingerprint, creating the visible effect of an invisible fingerprint. To achieve this contact angle, a surface with hydrophobic and oleophilic properties has been demonstrated to be desirable. In one approach to optimizing this effect, it was found that the water contact angle can be in the range of approximately 70 to 145 degrees, while the diiodomethane contact angle can be less than 45 degrees. In another approach, the water contact angle (WCA) and diiodomethane oil contact angle (OCA) of IFP are 80° and 35°, respectively. This results in water droplets beading up and oil droplets spreading on the substrate. Ultimately, controlling the wetting behavior of the substrate allows the refractive indexes of the substrate and surface to match, making fingerprints less visible. This matching phenomenon allows light to pass through the fingerprint without refraction or reflection, creating the optical illusion that fingerprint smudges are absent.

[0041] In exemplary embodiments, the article includes a substrate and a coating, such as a fingerprint-invisible coating or an IFP coating, deposited on a surface of the substrate. In some embodiments, the fingerprint-invisible coating comprises a non-fluorinated alkylsilane hydrolyzate polymer.

[0042] Illustratively, the substrate may be made of glass, polymer, glass ceramic, metal oxide, Plexiglas, or other materials, hi some embodiments, the substrate comprises glass, glass ceramic, wood, metal, metal oxide, or polymer.

[0043] The coating can be of a specific thickness, measured by distance from the surface of the substrate. In some embodiments, the coating is less than about 1000 nm. In some embodiments, the thickness is greater than 0.1 nm. In some embodiments, the thickness is from about 5 nm to about 300 nm.

[0044] Delta E is a measurement of the difference between clean or unused glass and glass with a fingerprint. Using a colorimeter (PCE instrument), Delta E is calculated by taking the square root of the equation: L2 + A2 + B2. This resulting E value is measured on unused glass and compared to a fingerprint after it has been applied or wiped to obtain the Delta E. By way of example, the lower the Delta E value, the less visible it is. In another embodiment, Delta Haze can be measured using spectrophotometry. In some embodiments, the relative enhancement is similar from a fingerprint-resistant coating to a fingerprint-invisible coating. By way of illustration, the Delta E is associated with fingerprint-resistant coatings such as perfluorinated silanes. By way of illustration, the lower the Delta E, the less visible a fingerprint is on the surface. Delta E can also be measured after wiping a surface to determine how well the fingerprint has been removed.

[0045] In some embodiments, the Delta E can be less than about 3, less than about 2, less than about 1, less than about 0.8, or less than about 0.5. In some embodiments, the Delta E is about 0.05, about 0.1, about 0.2, about 0.3, about 0.4, about 0.5, about 0.6, about 0.7, about 0.8, about 0.9, about 1, about 1.1, about 1.2, about 1.3, about 1.4, about 1.5, about 1.6, about 1.7, about 1.8, about 1.9, about 2, about 2.2, about 2.5, or about 3. In some embodiments, the Delta E is in the range of about 0.1 to about 2, about 0.1 to about 1.5, about 0.1 to about 1, about 0.2 to about 1, about 0.3 to about 1, or about 0.4 to about 0.9. In a second series of ranges, the Delta E can be from about 0.05 to about 1.2, from about 0.05 to about 0.9, from about 0.05 to about 0.8, or from about 0.05 to about 0.5.

[0046] In some embodiments, the fingerprint-invisible surface has an initial contact angle using diiodomethane (CHI), as measured according to the Examples. In some embodiments, the initial contact angle is less than about 60°, less than about 50°, less than about 45°, less than about 40°, less than about 35°, or less than about 30°. In some embodiments, the fingerprint-invisible surface has an initial contact angle of about 20°, about 21°, about 22°, about 23°, about 24°, about 25°, about 26°, about 27°, about 28°, about 29°, about 30°, about 31°, about 32°, about 33°, about 34°, about 35°, about 37°, about 40°, about 45°, about 50°, about 55°, or about 60°. In some embodiments, the initial contact angle of the non-fingerprint visible surface may range from about 20° to about 60°, from about 20° to about 50°, from about 20° to about 40°, from about 20° to about 35°, or from about 20° to about 30°.

[0047] In some embodiments, the non-visible fingerprint surface has an initial water contact angle, measured according to the Examples. In some embodiments, the initial water contact angle is greater than about 60°, greater than about 65°, greater than about 70°, greater than about 75°, greater than about 80°, greater than about 90°, or greater than about 100°. In some embodiments, the non-visible fingerprint surface has an initial water contact angle of about 60°, about 65°, about 70°, about 75°, about 76°, about 77°, about 78°, about 79°, about 80°, about 81°, about 82°, about 83°, about 84°, about 85°, about 86°, about 87°, about 88°, about 89°, about 90°, about 95°, about 100°, about 105°, about 110°, or about 115°. In some embodiments, the initial water contact angle of the non-visible fingerprint surface can range from about 60° to about 115°, from about 60° to about 110°, from about 70° to about 110°, from about 70° to about 95°, or from about 75° to about 95°.

[0048] In some embodiments, the non-fingerprint visible surface has a particular abrasion resistance as measured by water contact angle or contact angle after a particular number of cycles, as described in the Examples.

[0049] Illustratively, the fingerprint-invisible surface can have a specific contact angle after enduring about 1,500, about 3,000, about 4,500, or about 5,000 cycles, as described in the Examples. Illustratively, the contact angle after abrasion is less than about 60°, less than about 50°, less than about 45°, less than about 40°, less than about 35°, or less than about 30°. In some embodiments, the contact angle of the non-fingerprint visible surface after abrasion is about 20°, about 21°, about 22°, about 23°, about 24°, about 25°, about 26°, about 27°, about 28°, about 29°, about 30°, about 31°, about 32°, about 33°, about 34°, about 35°, about 37°, about 40°, about 45°, about 50°, about 55°, or about 60° after 1,500 cycles, about 3,000 cycles, about 4,500 cycles, or about 5,000 cycles. In some embodiments, the contact angle of the non-fingerprint visible surface after abrasion may range from about 20° to about 60°, about 20° to about 50°, about 20° to about 40°, about 20° to about 35°, or about 20° to about 30° after 1,500 cycles, about 3,000 cycles, about 4,500 cycles, or about 5,000 cycles.

[0050] Illustratively, the non-visible fingerprint surface may have a particular water contact angle after enduring about 1,500 cycles, about 3,000 cycles, about 4,500 cycles, or about 5,000 cycles, as described in the Examples. Illustratively, the water contact angle after abrasion may be greater than about 40°, greater than about 50°, greater than about 55°, or greater than about 60°. In some embodiments, the non-visible fingerprint surface has a water contact angle after abrasion of about 40°, about 50°, about 55°, about 60°, about 65°, about 70°, about 75°, about 80°, or about 85° after 1,500 cycles, 3,000 cycles, or 4,500 cycles. In some embodiments, the water contact angle of the non-visible fingerprint surface after abrasion can range from about 40° to about 85°, about 50° to about 85°, about 50° to about 80°, or about 60° to about 80° after 1,500 cycles, about 3,000 cycles, about 4,500 cycles, or about 5,000 cycles. In some embodiments, the non-visible fingerprint coating can maintain a water contact angle of at least 50° after 1,500 cycles of eraser abrasion.

[0051] In exemplary embodiments, the fingerprint-non-visible surface has a particular coefficient of friction. In some embodiments, the coefficient of friction is less than about 0.2 or less than about 0.15. In some embodiments, the coefficient of friction is about 0.08, about 0.09, about 0.1, about 0.11, about 0.12, about 0.13, about 0.14, or about 0.15. In some embodiments, the coefficient of friction is in the range of about 0.08 to about 0.15 or about 0.09 to about 0.13.

[0052] In some embodiments, the fingerprint-invisible coating is formed by applying a formulation for a fingerprint-invisible coating to a substrate, hi some embodiments, the formulation for a fingerprint-invisible coating includes a hydrolyzed alkylsilane.

[0053] Hydrolysates of alkylsilanes, sometimes referred to as hydrolysate polymers, can be formed by a process comprising contacting an alkylsilane with an acid or a base. In exemplary embodiments, the hydrolysates are formed by contacting an alkylsilane with an acid. In exemplary embodiments, the hydrolysates are formed by contacting an alkylsilane with an acid in a solvent. In some embodiments, the hydrolysate polymers are formed in the absence of an acid.

[0054] Acids that can be used to form the hydrolysate include mineral acids and organic acids. Exemplary mineral acids include hydrochloric acid, nitric acid, sulfuric acid, mixtures thereof, or other mineral acids known in the art. In some embodiments, the acid is nitric acid. In some embodiments, the acid is acetic acid.

[0055] In exemplary embodiments, the acid is present at a particular concentration. Illustratively, the acid is present at a concentration of at least about 0.01% by volume (about 0.01 vol%). The acid may be present at a concentration of about 0.01%, about 0.02%, about 0.03%, about 0.04%, about 0.05%, about 0.06%, about 0.07%, about 0.08%, about 0.09%, about 0.1%, about 0.11%, about 0.12%, about 0.13%, about 0.14%, about 0.15%, about 0.16%, about 0.17%, about 0.18%, about 0.19%, about 0. The acid may be present in an amount of about 2%, about 0.25%, about 0.3%, about 0.35%, about 0.4%, about 0.45%, about 0.5%, about 0.6%, about 0.7%, about 0.8%, about 0.9%, about 1%, about 1.5%, about 2%, about 3%, about 4%, about 5%, about 6%, about 7%, about 8%, about 9%, about 10%, about 15%, about 20%, about 25%, or about 50%. The acid may be present in a range of about 0.01% to about 50%, about 0.01% to about 15%, about 0.01% to about 10%, about 0.01% to about 5%, about 0.05% to about 5%, about 0.05% to about 3%, about 0.05% to about 1%, or about 0.05% to about 0.15%.

[0056] In some embodiments, the hydrolyzate is formed by contacting an alkylsilane with a base. Exemplary bases include potassium hydroxide.

[0057] In some embodiments, the hydrolyzate is formed by combining an alkylsilane with titanium butoxide, levacil, and an acid, which in some embodiments is acetic acid.

[0058] In exemplary embodiments, the step of forming the hydrolysate is carried out in a solvent. In some embodiments, the solvent comprises an alcohol, an organic solvent, or a mixture thereof. In some embodiments, the alcohol is an alkyl alcohol. In some embodiments, the alcohol is a C1-C 10 The alkyl alcohol is alkyl-OH or C1-C6 alkyl-OH. Exemplary alkyl alcohols include methanol, ethanol, propanol, isopropanol, or butanol. Exemplary organic solvents include chlorinated and non-chlorinated solvents. Exemplary chlorinated solvents include dichloromethane. In some embodiments, the solvent comprises water.

[0059] In some embodiments, the solvent is a mixture of water and an alcohol. In some embodiments, the alcohol is a C1-C 10 The water and alcohol are alkyl-OH or C1-C6 alkyl-OH. In some embodiments, the water and alcohol are present in a water to alcohol ratio of about 1:1000 to about 1000:1. In some exemplary embodiments, by controlling the ratio of the amount of water to alcohol in the solvent, it may be possible to produce hydrolyzates with varying molecular weights and varying conversion rates of starting material to final product. The conversion of monomer to oligomer or polymer can be determined by the water to ethoxy ratio of a reaction run at reflux overnight.

[0060] The solvent for forming the hydrolysate can have a particular pH, hi some embodiments, the pH is between 0 and 14 or between 6 and 8.

[0061] The contacting step, sometimes referred to as a polymerizing step, can be carried out for a specified time period. In some embodiments, the specified time period is the time period before quenching. In some embodiments, the contacting step is carried out for at least 3 minutes. In some embodiments, the contacting step is carried out for less than 4 hours. In exemplary embodiments, the contacting step is carried out for about 3 minutes, about 5 minutes, about 10 minutes, about 15 minutes, about 20 minutes, about 25 minutes, about 30 minutes, about 35 minutes, about 40 minutes, about 45 minutes, about 50 minutes, about 1 hour, about 2 hours, about 3 hours, or about 4 hours. In some embodiments, the polymerizing step can be carried out for about 0.1 hours to about 72 hours. In some embodiments, the polymerizing step can be carried out for about 0.1 hours to about 20 hours, or preferably about 12 hours.

[0062] The contacting step, sometimes referred to as polymerizing, can be carried out at a particular temperature or within a particular temperature range. In some embodiments, the step is carried out at the reflux temperature of the solvent. In some embodiments, the step is carried out at room temperature. In some embodiments, the step is carried out at a temperature below room temperature. In some embodiments, the step is carried out at a temperature of about -10°C until the solvent refluxes.

[0063] The method for forming the hydrolysate may include a step of quenching the contacting step. In exemplary embodiments, the step or quenching is carried out by adding an aqueous solution. In exemplary embodiments, the aqueous solution includes a base. Exemplary bases include sodium bicarbonate. In some embodiments, the aqueous solution is substantially free of base. In some embodiments, the method does not include a quenching step.

[0064] In an exemplary embodiment, the step of forming the hydrolysate includes a step of concentrating. In an exemplary embodiment, the step of concentrating is performed after the step of quenching. Alternatively, in an exemplary embodiment, the method does not include a step of quenching, and the step of concentrating occurs immediately after the step of forming / polymerizing. Illustratively, the step of concentrating is performed under vacuum.

[0065] In some embodiments, the method includes purifying the hydrolysate. In some embodiments, the purifying step includes washing the hydrolysate, for example, to remove any acid or catalyst that may be present. Illustratively, the washing can be done by washing with water.

[0066] In some embodiments, the alkylsilane has the following structural formula: (R A )3SiR B In some embodiments, each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 In some embodiments, each R is alkynyl. B is C1~C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 In some embodiments, -OC is alkynyl. 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, -OC 10 Alkynyl, C1-C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, C(O)OR 1 , -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—OCl-C6 alkyl)3—N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—OCl-C6 alkyl)3. In some embodiments, if present, each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, or -C1-C 10 Alkyl-O-C1~C 10 Alkyl, C1-C 10 Alkylaryl-O-C1~C 10 In some embodiments, R 1 C1 to C in 10 Alkyl, C1-C 10Each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl. Although 11-chloroundecyltriethoxysilane in some embodiments is described as "CLAS," it should be understood that such abbreviation is merely for brevity and is in no way intended to limit "CLAS" to 11-chloroundecyltriethoxysilane.

[0067] In some embodiments, R B is C1~C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Alkynyl. Examples include C1-C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom of an alkynyl can be independently selected from deuterium, halogen, —OH, —CN, —OR 1 , -CO2H, -C(O)OR 1 , -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(-O-C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, or -Si(-O-C1-C6 alkyl)3. Each R 1if present, is independently deuterium, C1-C6 alkyl, C2-C6 alkenyl, C2-C6 alkynyl, C3-C6 cycloalkyl, or —C1-C6 alkyl-O—C1-C6 alkyl, where each hydrogen atom of the C1-C6 alkyl is optionally replaced with hydroxy.

[0068] In some embodiments, R B is optionally substituted C6-C 20 In an exemplary embodiment, C-C alkyl. 20 Each hydrogen atom of an alkyl may be independently selected from the group consisting of halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 are independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl. In some embodiments, the alkylsilane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane, (11-undecylinic acid)(triethoxy)silane, (hydroxyheptyl)(triethoxy)silane, and (11-phosphoundecyl)(triethoxy)silane. In some embodiments, the alkylsilane is 11-chloroundecyltriethoxysilane.

[0069] Illustratively, the halogen may be chloro, bromo, or iodo. In some embodiments, the alkylsilane includes a halogen but does not include a fluoro.

[0070] In some embodiments, the alkylsilane is difunctional. Illustratively, a difunctional silane can be considered a crosslinking silane or a chain extender in embodiments having more than one alkylsilane. Exemplary difunctional alkylsilanes include haloalkylsilanes, bisalkylsilanes, bisalkoxysilanes, aminoalkylsilanes, hydroxyalkylsilanes, and phosphate alkylsilanes. Exemplary bisalkylsilanes include bistriethoxyoctylsilane and bis(trimethoxysilyl)4-oxa-8-azundecan-6-ol. Exemplary haloalkylsilanes include chloroundecylsilane and chlorohexylsilane. Exemplary aminoalkylsilanes include aminoundecylsilane, N-2-aminoethyl-11-aminoundecyltriethoxysilane, and N-6-aminohexylaminomethyltriethoxysilane. Exemplary hydroxyalkylsilanes include OH-decyltriethoxysilane. Exemplary phosphate alkylsilanes include phosphate undecyltriethoxysilane.

[0071] Exemplary crosslinked silanes include those selected from the group consisting of formulas (I)-(IV): (I)(SiX n )-Y 1 , (II)(SiX n )-Y 2 -(SiX n ), (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and (IV)(SiX n )-(SiX n )-Y 4 -(SiX n )-(SiX n )

[0072] In some embodiments, Y 1 (C2~C 30) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (I) is 1 In some embodiments, Y 2 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (II) is 2 In some embodiments, Y 3 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (III) is 3 In some embodiments, Y 4 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (IV) is 4In some embodiments, each X is independently a monovalent leaving group selected from halogen, (C1-C6)alkoxy, (C2-C6)carboxy, (C1-C6)oximo, and (C1-C6)arylalkoxy. In some embodiments, n is an integer between 1 and 3. Adding a chain extender, such as a BIS or TRIS silane, in various ratios to an alkyl silane, such as 11-chloroundecyltriethoxysilane, can potentially increase the molecular weight of the final polymer and improve the durability of the final product. The tunability of this approach allows for customizable 11-chloroundecyltriethoxysilane hydrolysates, which can be tailored to improve performance. In some embodiments, the final result is an IFP coating, which has the potential to be both high-performance and easily mass-produced. An exemplary BIS silane is 1,2-bis(triethoxysilyl)ethane. Although the 1,2-bis(triethoxysilyl)ethane of some embodiments is referred to as "BIS," it should be understood that such abbreviation is merely for brevity and is in no way intended to limit "BIS" to 1,2-bis(triethoxysilyl)ethane. An exemplary TRIS silane is 1,1,2-tris(triethoxysilyl)ethane. Although the 1,1,2-tris(triethoxysilyl)ethane of some embodiments is referred to as "TRIS," it should be understood that such abbreviation is merely for brevity and is in no way intended to limit "TRIS" to 1,1,2-tris(triethoxysilyl)ethane.

[0073] In some embodiments, the contacting step further comprises an alkoxysiloxane. In some embodiments, the alkoxysilane is a trialkoxysiloxane. In some embodiments, the dialkylsiloxane is a vinyl-terminated dialkylsiloxane having the formula (R c O)3SiH, where R cis an alkyl group. In some embodiments, the siloxane is an alkyl siloxane. In some embodiments, the alkoxy siloxane is an alkoxy polydimethyl siloxane. In some embodiments, the alkoxy siloxane is a trialkoxy polydimethyl siloxane.

[0074] In exemplary embodiments, the trialkoxysiloxane is formed by reacting a trialkoxysilane with a commercially available siloxane in the presence of a catalyst. Exemplary siloxanes include polydimethylsiloxanes available from Gelest. In some embodiments, the catalyst is a platinum catalyst.

[0075] Illustratively, the formed hydrolysate, sometimes referred to as a hydrolysate polymer, comprises higher molecular weight species compared to the alkylsilane. In some embodiments, the formed hydrolysate comprises species having a molecular weight of at least 1,000 Da, at least about 2,000 Da, or at least about 3,000 Da. In some embodiments, the formed hydrolysate comprises species of about 1,000 Da, about 1,500 Da, about 2,000 Da, about 2,500 Da, about 3,000 Da, about 3,500 Da, about 4,000 Da, about 4,500 Da, about 5,000 Da, about 5,500 Da, about 6,000 Da, about 6,500 Da, about 7,000 Da, about 7,500 Da, about 8,000 Da, about 9,000 Da, or about 10,000 Da. In some embodiments, the hydrolysate polymers formed include species of at least about 300 Da or at least about 500 Da.

[0076] In some embodiments, the hydrolysate polymer has a weight average molecular weight (Mw) of less than about 100,000 Da or less than about 50,000 Da. In some embodiments, the hydrolysate polymer has a weight average molecular weight (Mw) of at least about 300 Da, at least about 500 Da, at least about 600 Da, or at least about 1,000 Da. In some embodiments, the hydrolysate polymer has a weight average molecular weight (Mw) in a first set of ranges: from about 300 Da to about 100,000 Da, from about 500 Da to about 100,000 Da, from about 500 Da to about 50,000 Da, from about 500 Da to about 25,000 Da, from about 500 Da to about 10,000 Da, or from about 500 Da to about 5,000 Da. In some embodiments, the hydrolysate polymer has a weight average molecular weight (Mw) in a second set of ranges from about 500 Da to about 100,000 Da, from about 1,000 Da to about 100,000 Da, from about 10,000 Da to about 100,000 Da, from about 15,000 Da to about 100,000 Da, or from about 30,000 Da to about 100,000 Da.

[0077] In some embodiments, the hydrolysate polymer has a number average molecular weight (Mn) of less than about 100,000 Da or less than about 50,000 Da. In some embodiments, the hydrolysate polymer has a number average molecular weight (Mn) of at least about 300 Da, at least about 500 Da, at least about 600 Da, or at least about 1,000 Da. In some embodiments, the hydrolysate polymer has a number average molecular weight (Mn) in a first set of ranges: from about 300 Da to about 100,000 Da, from about 500 Da to about 100,000 Da, from about 500 Da to about 50,000 Da, from about 500 Da to about 25,000 Da, from about 500 Da to about 10,000 Da, or from about 500 Da to about 5,000 Da. In some embodiments, the hydrolysate polymer has a number average molecular weight (Mn) in a second set of ranges from about 500 Da to about 100,000 Da, from about 1,000 Da to about 100,000 Da, from about 10,000 Da to about 100,000 Da, from about 15,000 Da to about 100,000 Da, or from about 30,000 Da to about 100,000 Da.

[0078] In some embodiments, the hydrolysate polymer has a polydispersity index (Mw / Mn) of at least about 1.1 or at least about 1.2. In some embodiments, the hydrolysate polymer has a polydispersity index (Mw / Mn) of less than about 1.8 or less than about 1.7. In some embodiments, the hydrolysate polymer has a polydispersity index of about 1.1, about 1.2, about 1.3, about 1.4, about 1.5, about 1.6, about 1.7, or about 1.8.

[0079] In some exemplary embodiments, the hydrolysate polymer may include some or all of blocks A through F, as shown below.

[0080] [ka] where R A and R Bis defined above. m, n, o, p, q, and r are each independently an integer. Illustratively, each integer may independently be from 0 to 500. Illustratively, in some embodiments, some or all of blocks A through F are present in the hydrolysate polymer. For example, but not limited to, blocks A, F, and D can be combined to form the following exemplary structures:

[0081] [ka] Here, an example of each block 1 / 2 combine to connect two silicon atoms. While the above structure is linear as shown, the blocks can also be joined into three-dimensional shapes, including but not limited to, as shown in the examples below.

[0082] [ka] In exemplary embodiments, it is contemplated that the hydrolysate polymer comprises linear stretches of blocks selected from the group consisting of A, B, C, D, E, F, and combinations thereof, and branched segments of blocks selected from the group consisting of A, B, C, D, E, F, and combinations thereof. Without being bound by theory, the amount of water present during polymerization may affect the degree of branching and polymerization.

[0083] The concentration of the hydrolysate polymer in the formulation for the fingerprint-invisible coating may be a specific concentration in a solvent. In some embodiments, the hydrolysate is present at a concentration of at least 1 g / L. In some embodiments, the hydrolysate is present at a concentration of about 1 g / L to about 10 g / L, 1 g / L to about 6 g / L, about 1 g / L to about 5 g / L, about 2 g / L to about 5 g / L, or about 3 g / L to about 5 g / L. In some embodiments, the hydrolysate may be present at a concentration of about 1 g / L, about 2 g / L, about 3 g / L, about 3.25 g / L, about 3.5 g / L, about 3.75 g / L, about 4 g / L, about 4.25 g / L, about 4.5 g / L, about 5 g / L, about 5.5 g / L, about 6 g / L, about 7 g / L, about 8 g / L, about 9 g / L, or about 10 g / L. In some embodiments, the hydrolysate is at a concentration of about 0.01 mg / L to about 100 g / L.

[0084] In some embodiments, the formulation for the fingerprint-invisible coating includes a solvent. In some embodiments, the solvent is an organic solvent. In some embodiments, the solvent includes water, an alcohol, or a mixture thereof. In some embodiments, the alcohol is a C1-C6 alkyl-OH. In some embodiments, the solvent is methanol, ethanol, propanol, butanol, pentanol, hexanol, or a combination thereof. In exemplary embodiments, the formulation for the fingerprint-invisible coating is substantially acid-free. In exemplary embodiments, the solvent is substantially acid-free.

[0085] As an illustration, a formulation for a fingerprint-invisible surface can be applied to a substrate to form the fingerprint-invisible surface by a specific method. In some embodiments, the method for forming a fingerprint-invisible coating on a substrate includes a coating step. In some embodiments, the method includes a curing step. In some embodiments, the method includes a coating step and a curing step. In some exemplary embodiments, when the hydrolysate polymer is cured on a surface, the hydrolysate polymer bonds to the surface of the substrate, e.g., to free hydroxy groups on the surface.

[0086] In some embodiments, the applying step is carried out by dipping, wiping, spraying, chemical vapor deposition (CVD), or physical vapor deposition (PVD) of a formulation for a fingerprint-invisible coating onto the surface of the substrate.

[0087] In some embodiments, a method for forming a fingerprint-invisible coating on a substrate includes applying a fingerprint-invisible coating formulation to a surface of the substrate by physical vapor deposition. Illustratively, the applying step can be performed by thermal evaporation. In some embodiments, the method includes curing the formulation on the surface of the substrate. In some embodiments, the method includes cleaning the surface of the substrate. In some embodiments, the cleaning step is performed before the applying step. In some embodiments, the formulation is in the form of pellets. In some embodiments, the method includes forming pellets of the formulation. In some exemplary embodiments, the pellet-forming step includes contacting steel wool or copper foam with the hydrolysate.

[0088] Illustratively, the curing step can be carried out at elevated temperatures or at room temperature. In some embodiments, the curing step is carried out at room temperature. In some embodiments, the curing step is carried out at at least about 70°C, at least about 80°C, at least about 90°C, or at least about 100°C. In some embodiments, the curing step is carried out at a temperature of about 80°C, about 90°C, about 100°C, about 110°C, about 120°C, about 125°C, about 130°C, or about 140°C. In some embodiments, the curing step is carried out at a temperature of 20°C or more and 250°C or less. In some embodiments, when curing is carried out by heating, the hydrolysate polymer may further condense with itself to form higher molecular weight species compared to the molecular weight species present in the formulation.

[0089] In some embodiments, the curing step is carried out for a period of time to harden the formulation, which may depend on the temperature used in the curing step. In some embodiments, the curing step is carried out overnight. In some embodiments, the curing step is carried out for at least about 5 minutes, at least about 10 minutes, or at least about 30 minutes. In some embodiments, the curing step is carried out for about 10 minutes, about 15 minutes, about 20 minutes, about 25 minutes, about 30 minutes, about 45 minutes, about 1 hour, about 2 hours, about 3 hours, about 4 hours, about 6 hours, about 12 hours, or overnight. In some embodiments, the curing step is carried out at a temperature of about 120°C for about 10 minutes. In some embodiments, the curing step is carried out at a temperature of about 80°C for about 1 hour. In some embodiments, the curing step is carried out overnight at room temperature. In some embodiments, the curing step is carried out at a temperature of about 120°C for about 30 minutes. In some embodiments, the curing step is carried out for at least 0.1 hour and up to 48 hours.

[0090] In some embodiments, the method includes activating a surface of the substrate by exposing the surface to a plasma of at least one gas selected from the group consisting of an inert gas, N2, O2, and a mixture of at least two of said gases.

[0091] In exemplary embodiments, the formulation for the fingerprint-invisible coating is deposited by dipping, spraying, thermal CVD (chemical vapor deposition), or physical vapor deposition (PVD) under conditions that allow for an RMS (root mean square) surface roughness of between 5 and 100 nm. In exemplary embodiments, an RMS (root mean square) surface roughness of between 5 and 10 nm can be obtained.

[0092] Although only a few exemplary embodiments have been described in detail above, those skilled in the art will readily appreciate that many modifications are possible in the exemplary embodiments without materially departing from the novel teachings and advantages. The first set of numbered clauses below encompass intended, non-limiting embodiments.

[0093] Article 1. 1. A fingerprint-invisible surface comprising a fingerprint-invisible coating made by a method comprising the steps of forming a low molecular weight alkyl silane hydrolysate;

[0094] applying a formulation containing the low molecular weight alkylsilane hydrolysate to a surface of a substrate;

[0095] A portion of the low molecular weight alkylsilane hydrolysate has a molecular weight of about 5,000 Da.

[0096] Article 2. 10. The fingerprint-invisible surface of claim 1, wherein the forming step includes contacting an alkylsilane with an acid.

[0097] Article 3. The alkylsilane has the formula: (R A )3SiRB , is an alkylsilane of:

[0098] In the formula, each R A are independently -OC1-C6 alkyl, -OC2-C6 alkenyl, or -OC3-C6 alkynyl; and R B is C1~C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Alkynyl; where, -OC1-C6 alkyl, -OC1-C6 alkenyl, -OC1-C6 alkynyl; C1-C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, -C(O)OR 1 , -C(O)NH2, C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and Here, each R 1are independently deuterium, C1-C6 alkyl, C2-C6 alkenyl, C2-C6 alkynyl, C3-C6 cycloalkyl, or -C1-C6 alkyl-O-C1-C6 alkyl, wherein each hydrogen atom in the C1-C6 alkyl is optionally substituted with hydroxy.

[0099] Article 4. In the above formula, R A The fingerprint-invisible surface according to any one or combination of the preceding clauses, wherein -OC1-C6 alkyl is

[0100] Article 5. In the above formula, R B is C6~C 20 The fingerprint-invisible surface of any one or combination of the preceding clauses, wherein the surface is alkyl.

[0101] Article 6. In the above formula, R B is C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 wherein each of the groups is independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl.

[0102] Article 7. The fingerprint-invisible surface of any one of the preceding clauses or combinations thereof, wherein the alkylsilane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecylated)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; and (phosphoundecyl)(triethoxy)silane.

[0103] Article 8. The fingerprint-invisible surface according to any one of the preceding clauses or combinations of clauses, wherein the alkylsilane is 11-chloroundecyltriethoxysilane.

[0104] Article 9. 10. The fingerprint-non-visible surface of claim 1, wherein the acid comprises a mineral acid.

[0105] Article 10. 4. The fingerprint-invisible surface of claim 1, wherein the mineral acid is hydrochloric acid, nitric acid, sulfuric acid, or a mixture thereof.

[0106] Article 11. The fingerprint-invisible surface of any one of the preceding clauses or combination of clauses, wherein the acid is present in a concentration of about 0.01% to about 10%.

[0107] Article 12. 10. The fingerprint-invisible surface of claim 1, wherein the contacting step is carried out for at least about 5 minutes.

[0108] Article 13. 10. The fingerprint-invisible surface of claim 1, wherein the contacting step is performed for less than about 3 hours.

[0109] Article 14. The non-fingerprint visible surface of any one or combination of the preceding clauses, wherein the contacting step occurs for about 10 minutes to about 2 hours.

[0110] Article 15. The non-fingerprint visible surface of any one or combination of the preceding clauses, wherein the contacting step occurs for about 10 minutes to about 1 hour.

[0111] Article 16. 10. The non-fingerprint visible surface of claim 1, wherein the contacting step is performed for about 10 minutes to about 30 minutes.

[0112] Article 17. The non-fingerprint visible surface of any one of the preceding clauses or combination of clauses, wherein the contacting step further includes a dialkylsiloxane.

[0113] Article 18. 18. The fingerprint-invisible surface of clause 17, wherein the dialkylsiloxane is capped with a trialkoxysilane.

[0114] Article 19. The dialkylsiloxane may be prepared by reacting a vinyl-terminated dialkylsiloxane with a compound of the formula (R c O)3SiH, where R c 19. The fingerprint-invisible surface according to clause 17 or 18, wherein: is an alkyl group.

[0115] Article 20. 20. The fingerprint-less surface of any one of clauses 19, wherein the catalyst comprises platinum.

[0116] Article 21. In the above formula, Rc 21. The fingerprint-invisible surface according to clause 19 or 20, wherein R is methyl, ethyl, or propyl.

[0117] Article 22. 22. The fingerprint-invisible surface of any one of clauses 17 to 21, wherein the dialkylsiloxane has a molecular weight of at least 3,000 Da.

[0118] Article 23. 23. The fingerprint-invisible surface of any one of clauses 17 to 22, wherein the dialkylsiloxane comprises polydimethylsiloxane (PDMS).

[0119] Article 24. The fingerprint-invisible surface according to any preceding clause or combination of clauses, wherein the low molecular weight alkyl silane hydrolyzate does not contain fluoro.

[0120] Article 25. The fingerprint-free surface of any preceding clause or combination of clauses, wherein the formulation is acid-free.

[0121] Article 26. 26. The fingerprint-invisible surface of clause 25, wherein the acid is a mineral acid.

[0122] Article 27. 27. The fingerprint-non-visible surface of clause 26, wherein the mineral acid is hydrochloric acid, nitric acid, sulfuric acid, or a mixture thereof.

[0123] Article 28. 4. The non-fingerprint visible surface of claim 1, wherein the contacting step is carried out in a solvent.

[0124] Article 29. 29. The fingerprint-invisible surface of claim 28, wherein the solvent is a mixture of an organic solvent and an alcohol.

[0125] Article 30. 30. The fingerprint-non-visible surface of claim 29, wherein the organic solvent is a chlorinated solvent.

[0126] Article 31. 31. The fingerprint-invisible surface according to clause 30, wherein the chlorinated solvent is chloroform or dichloromethane.

[0127] Article 32. 32. The fingerprint-non-visible surface according to any one of clauses 29 to 31, wherein the alcohol is an alkyl alcohol.

[0128] Article 33. 33. The fingerprint-invisible surface of claim 32, wherein the alkyl alcohol is methanol, ethanol, propanol, butanol, or pentanol.

[0129] Article 34. 34. The fingerprint-invisible surface of clause 33, wherein the propanol is isopropanol or n-propanol.

[0130] Article 35. 36. The fingerprint-non-visible surface of any one of clauses 29 to 35, wherein the mixture is from about 5:1 organic solvent:alcohol to about 15:1 organic solvent:alcohol.

[0131] Article 36. 36. The fingerprint-non-visible surface of any one of clauses 29 to 35, wherein the mixture is from about 7:1 organic solvent:alcohol to about 12:1 organic solvent:alcohol.

[0132] Article 37. 36. The fingerprint-non-visible surface of any one of clauses 29 to 35, wherein the mixture is about 8:1 organic solvent:alcohol or about 10:1 organic solvent:alcohol.

[0133] Article 38. 2. The fingerprint-invisible surface of claim 1, wherein the applying step comprises chemical vapor deposition (CVD) or physical vapor deposition (PVD) of the formulation.

[0134] Article 39. 10. The fingerprint-invisible surface of claim 1, wherein the formulation is a liquid formulation and the applying step comprises spraying the liquid formulation onto the surface.

[0135] Article 40. 10. The non-visible fingerprint surface of claim 1, wherein the non-visible fingerprint surface has an initial contact angle with diiodomethane of less than about 45° and an initial contact angle with water of more than about 65°.

[0136] Article 41. 2. The fingerprint-invisible surface of claim 1, wherein the substrate comprises at least one material selected from the group consisting of glass, metal oxide, and acrylic polymer.

[0137] Article 42. 10. The fingerprint-invisible surface of any one of the preceding clauses or combinations thereof, wherein the fingerprint-invisible surface has a thickness ranging from about 5 nm to about 300 nm.

[0138] Article 43. 10. The fingerprint-invisible surface of any one or combination of the preceding clauses, wherein the fingerprint-invisible surface has an initial contact angle with diiodomethane of less than about 50°.

[0139] Article 44. 10. The non-visible fingerprint surface of any one of the preceding clauses or a combination of clauses, wherein the non-visible fingerprint surface has an initial contact angle of less than about 45°.

[0140] Article 45. 10. The non-visible fingerprint surface of any one of the preceding clauses or a combination of clauses, wherein the non-visible fingerprint surface has an initial contact angle of less than about 35°.

[0141] Article 46. 10. The non-visible fingerprint surface of any one or combination of the preceding clauses, wherein the non-visible fingerprint surface has an initial water contact angle of greater than about 65°.

[0142] Article 47. 10. The non-visible fingerprint surface of any one of the preceding clauses or a combination of clauses, wherein the non-visible fingerprint surface has an initial water contact angle of about 70° to about 90°.

[0143] Article 48. 10. The non-visible fingerprint surface of any one or combination of the preceding clauses, wherein the non-visible fingerprint surface is substantially fluoride-free.

[0144] Article 49. 10. The non-visible fingerprint surface of any one of the preceding clauses or a combination of clauses, wherein the non-visible fingerprint surface has an initial water contact angle of about 70° to about 90°.

[0145] Article 50. 10. The fingerprint-invisible surface of any one or combination of the preceding clauses, wherein the fingerprint-invisible surface has a coefficient of friction of less than about 0.15.

[0146] Article 51. 10. The fingerprint-invisible surface of any one or combination of the preceding clauses, wherein the fingerprint-invisible surface has a coefficient of friction of less than about 0.13.

[0147] Article 52. 10. The non-visible fingerprint surface of any one or combination of the preceding clauses, wherein the non-visible fingerprint surface has a coefficient of friction of about 0.05 to about 0.13.

[0148] Article 53. A formulation for a fingerprint-invisible coating, said formulation comprising a low molecular weight alkyl silane hydrolyzate and a solvent.

[0149] Article 54. The low molecular weight alkylsilane hydrolyzate has the following formula: (R A )3SiR B , formed from an alkylsilane of

[0150] In the formula, each R A are independently -OC1-C6 alkyl, -OC1-C6 alkenyl, or -OC1-C6 alkynyl; and R B is C1~C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Alkynyl; where, -OC1-C6 alkyl, -OC1-C6 alkenyl, -OC1-C6 alkynyl; C1-C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -OC1~C6 alkyl, -CO2H, C(O)OC1~C6 alkyl, -C(O)NH2, C(O)NH(C1~C6 alkyl), -C(O)N(C1~C6 alkyl)2, SC1~C6 alkyl, S(O)C1~C6 alkyl, -S(O)2C1~C6 alkyl, -S(O)NH(C1~C6 alkyl), -S(O)2NH(C1~C6 alkyl), -S(O)N(C1~C6 alkyl)2, -S(O)2N(C1~C6 alkyl)2, -NH2, NH(C1~C6 alkyl), -N(H)C1~C6 alkyl-NH2, -N(H)C1~C6 alkyl-Si(-OC1~C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—OCl-C6 alkyl)3—N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—OCl-C6 alkyl)3; and wherein R 1 are independently deuterium, C1-C6 alkyl, C2-C6 alkenyl, C2-C6 alkynyl, C3-C6 cycloalkyl, or -C1-C6 alkyl-O-C1-C6 alkyl, wherein each hydrogen atom in the C1-C6 alkyl is optionally replaced with hydroxy.

[0151] Article 55. R A 55. The composition of claim 54, wherein is —OC1-C6 alkyl.

[0152] Article 56. In the above formula, R B C6~C 20 56. The composition of claim 54 or 55, wherein the alkyl is alkyl.

[0153] Article 57. In the above formula, R B C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 is independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl.

[0154] Article 58. 58. The formulation of any one of clauses 54-57, or combinations thereof, wherein the alkyl silane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane, (11-undecylinic acid)(triethoxy)silane, (hydroxyheptyl)(triethoxy)silane, (11-phosphoundecyl)(triethoxy)silane.

[0155] Article 59. 59. The formulation of any one or combination of clauses 54 to 58, wherein the alkylsilane is 11-chloroundecyltriethoxysilane.

[0156] Article 60. 60. The formulation of any one or combination of clauses 53-59, wherein the low molecular weight alkylsilane hydrolyzate comprises a dialkylsiloxane.

[0157] Article 61. 61. The formulation of clause 60, wherein the dialkylsiloxane comprises polydimethylsiloxane (PDMS).

[0158] Article 62. 62. The formulation of any one of clauses 53 to 61 or a combination thereof, wherein the formulation is acid-free.

[0159] Article 63. 63. The formulation of clause 62, wherein the acid is a mineral acid.

[0160] Article 64. 64. The formulation of clause 63, wherein the mineral acid is hydrochloric acid, nitric acid, sulfuric acid, or a mixture thereof.

[0161] Article 65. 1. A method for forming a fingerprint-invisible coating on a substrate, the method comprising:

[0162] applying a fingerprint-invisible coating formulation to the surface of a substrate; and

[0163] The method includes curing the formulation for the non-visible fingerprint coating on the surface of the substrate to form the non-visible fingerprint coating.

[0164] Article 66. 66. The method of claim 65, wherein the formulation for the fingerprint-invisible coating comprises a low molecular weight alkyl silane hydrolyzate.

[0165] Article 67. 67. The method of claim 65 or 66, wherein the low molecular weight alkylsilane hydrolysate is prepared by contacting an alkylsilane with an acid.

[0166] Article 68. The alkylsilane has the formula: (R A )3SiR B , is an alkylsilane of:

[0167] In the formula, each R A are independently -OC1-C6 alkyl, -OC2-C6 alkenyl, or -OC2-C6 alkynyl; and R B is C1~C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Alkynyl; where, -OC1-C6 alkyl, -OC1-C6 alkenyl, -OC1-C6 alkynyl; C1-C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, -C(O)OC1-C6 alkyl, -C(O)NH2, C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, -S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1)C1-C6 alkyl-Si(—OCl-C6 alkyl)3—N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—OCl-C6 alkyl)3; and wherein R 1 are independently deuterium, C1-C6 alkyl, C2-C6 alkenyl, C2-C6 alkynyl, C3-C6 cycloalkyl, or -C1-C6 alkyl-O-C1-C6 alkyl, wherein each hydrogen atom in the C1-C6 alkyl is optionally replaced with hydroxy.

[0168] Article 69. 69. The method of any one or combination of clauses 65-68, wherein the fingerprint non-visible coating has an initial contact angle with oil of at least about less than 50°.

[0169] Article 70. 70. The method of any one or combination of clauses 65-69, wherein the fingerprint non-visible coating has an initial contact angle with oil of at least about 45° or less.

[0170] Article 71. 71. The method of any one or combination of clauses 65-70, wherein the fingerprint non-visible coating has an initial water contact angle of greater than about 65°.

[0171] Article 72. 72. The method of any one or combination of clauses 65-71, wherein the fingerprint non-visible coating has an initial water contact angle of about 70° to about 90°.

[0172] Article 73. 73. The method of any one or combination of clauses 65 to 72, wherein the method comprises activating a surface of the substrate by exposing the surface to a plasma of at least one gas selected from the group consisting of an inert gas, N2, O2, and a mixture of at least two of said gases.

[0173] Article 74. 74. The method of any one or combination of clauses 65 to 73, wherein the applying step is performed by chemical vapor deposition (CVD), physical vapor deposition (PVD), dipping, wiping, or spraying the formulation for the fingerprint invisible coating onto the surface of the substrate.

[0174] Article 75. 75. The method of any one or combination of clauses 65 to 74, wherein the formulation is acid-free.

[0175] Article 76. 76. The method of clause 75, wherein the acid is a mineral acid.

[0176] Article 77. 77. The method of claim 76, wherein the mineral acid is hydrochloric acid, nitric acid, sulfuric acid, or a mixture thereof.

[0177] Article 78. 1. A method for forming a hydrolysate, the method comprising:

[0178] The following formula: (R A )3SiR B , with an acid,

[0179] In the formula, each R A are independently -OC1-C6 alkyl, -OC2-C6 alkenyl, or -OC2-C6 alkynyl; and R B is C1~C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20 Alkynyl; where, -OC1-C6 alkyl, -OC1-C6 alkenyl, -OC1-C6 alkynyl; C1-C 20 Alkyl, C2-C 20 Alkenyl, or C2-C 20Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, -C(O)OC1-C6 alkyl, -C(O)NH2, C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, -S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—OCl-C6 alkyl)3—N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—OCl-C6 alkyl)3; and wherein R 1 are independently deuterium, C1-C6 alkyl, C2-C6 alkenyl, C2-C6 alkynyl, C3-C6 cycloalkyl, or -C1-C6 alkyl-O-C1-C6 alkyl, wherein each hydrogen atom in the C1-C6 alkyl is optionally replaced with hydroxy; and

[0180] quenching the contacting step;

[0181] The method wherein the hydrolysate comprises the alkylsilane and a species having a molecular weight of about 5,000 Da.

[0182] Article 79. In the above formula, R A 79. The method according to clause 78, wherein is -OC1-C6 alkyl.

[0183] Article 80. In the above formula, R B is C6~C 2080. The method of claim 78 or 79, wherein the alkyl is alkyl.

[0184] Article 81. In the above formula, R B is C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 is independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl.

[0185] Article 82. 82. The method of any one or combination of clauses 78-81, wherein the alkyl silane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecylated)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; (phosphoundecyl)(triethoxy)silane.

[0186] Article 83. 83. The method of any one or combination of clauses 78 to 82, wherein the alkylsilane is 11-chloroundecyltriethoxysilane.

[0187] Article 84. 84. The method of any one or combination of clauses 78 to 83, wherein the acid comprises a mineral acid.

[0188] Article 85. 85. The method of claim 84, wherein the mineral acid is hydrochloric acid, nitric acid, sulfuric acid, or a mixture thereof.

[0189] Article 86. 86. The method of any one or combination of clauses 78 to 85, wherein the acid is present in a concentration of about 0.01% to about 10%.

[0190] Article 87. 87. The method of any one or combination of clauses 78-86, wherein said contacting step is carried out for at least about 5 minutes.

[0191] Article 88. 88. The method of any one or combination of clauses 78 to 87, wherein said contacting step is carried out for less than about 3 hours.

[0192] Article 89. 89. The method of any one or combination of clauses 78 to 88, wherein said contacting step occurs for about 10 minutes to about 2 hours.

[0193] Article 90. 89. The method of any one or combination of clauses 78 to 88, wherein said contacting step occurs for about 10 minutes to about 1 hour.

[0194] Article 91. 89. The method of any one or combination of clauses 78 to 88, wherein said contacting step is carried out for about 10 minutes to about 30 minutes.

[0195] Article 92. 92. The method of any one or combination of clauses 78-91, wherein said contacting step further includes a dialkylsiloxane.

[0196] Article 93. 93. The fingerprint-invisible surface of clause 92, wherein the dialkylsiloxane is capped with a trialkoxysilane.

[0197] Article 94. The dialkylsiloxane may be prepared by reacting a vinyl-terminated dialkylsiloxane with a compound of the formula (R c O)3SiH, where R c 94. The method of claim 92 or 93, wherein:

[0198] Article 95. 95. The fingerprint-invisible surface of clause 94, wherein the catalyst comprises platinum.

[0199] Article 96. In the above formula, R c 95. The fingerprint-invisible surface of clause 93 or 94, wherein is methyl, ethyl, or propyl.

[0200] Article 97. 97. The fingerprint-invisible surface of any one of clauses 92 to 96 or a combination thereof, wherein the dialkylsiloxane has a molecular weight of at least 3,000 Da.

[0201] Article 98. 98. The fingerprint-invisible surface of any one of clauses 92 to 97 or a combination thereof, wherein the dialkylsiloxane comprises polydimethylsiloxane (PDMS).

[0202] Article 99. 1. A method for forming a fingerprint-invisible coating on a substrate, the method comprising:

[0203] applying a fingerprint-invisible coating formulation to the surface of a substrate by physical vapor deposition; and

[0204] The method includes curing the formulation for the non-visible fingerprint coating on the surface of the substrate to form the non-visible fingerprint coating.

[0205] Article 100. 99. The method of claim 99, wherein the formulation for the fingerprint-invisible coating comprises a low molecular weight alkyl silane hydrolyzate.

[0206] Article 101. 101. The method of claim 99 or 100, wherein the formulation is acid-free.

[0207] Article 102. 102. The method of any one or combination of clauses 99-101, wherein the method further comprises cleaning the surface of the substrate.

[0208] Article 103. 103. The method of claim 102, wherein the cleaning step occurs before the applying step.

[0209] Article 104. 104. The method of any one of clauses 99 to 103 or combinations thereof, wherein the formulation is in the form of pellets.

[0210] Article 105. 100. The method of clause 99, wherein the method includes forming the pellet.

[0211] Article 106. 106. The method of claim 105, wherein the step of forming a pellet includes contacting steel wool or copper foam with the fingerprint non-visible coating formulation.

[0212] Article 107. 107. The method of any one or combination of clauses 99-106, wherein the applying step is performed by thermal evaporation.

[0213] The second set of clauses, numbered below, includes the following contemplated, non-limiting embodiments:

[0214] Article 1. An article,

[0215] A substrate;

[0216] a fingerprint-invisible coating laminated to the substrate; The article, wherein the fingerprint-invisible coating comprises a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da.

[0217] Article 2. An article,

[0218] A substrate;

[0219] a fingerprint-invisible coating laminated to the substrate; the fingerprint-invisible coating comprises a non-fluorinated alkylsilane hydrolyzate polymer;

[0220] The article, wherein the fingerprint-invisible coating has a thickness of less than 1000 nm and greater than 0.1 nm.

[0221] Article 3. 10. The article of any preceding clause, wherein the fingerprint-invisible coating comprises a surface having an initial contact angle using diiodomethane of less than about 50° and / or an initial water contact angle of more than about 65°.

[0222] Article 4. 10. The article of any preceding clause, wherein the substrate comprises a material selected from the group consisting of glass, glass ceramic, wood, metal, metal oxide, or polymer.

[0223] Article 5. 10. The article of any preceding clause, wherein the fingerprint-invisible coating has a thickness ranging from about 0.1 nm to about 1000 nm.

[0224] Article 6. 10. The article of any preceding clause, wherein the fingerprint-invisible coating has a coefficient of friction of less than about 0.15.

[0225] Article 7. 10. The article of any preceding clause, wherein the fingerprint-invisible coating is capable of maintaining a water contact angle of at least 50 degrees after 1500 cycles of eraser abrasion.

[0226] Article 8. The non-fluorinated alkylsilane hydrolyzate polymer has the following structural formula: (R A )3SiR B and the alkylsilane is formed from an alkylsilane having the formula:

[0227] During the ceremony:

[0228] Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl;

[0229] Each R B is C1~C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 is alkynyl;

[0230] -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, -OC 10 Alkynyl, C1-C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1, -CO2H, C(O)OR 1 , -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and

[0231] Each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, or -C1-C 10 Alkyl-O-C1~C 10 alkyl;

[0232] C1~C 10 Alkylaryl-O-C1~C 10 alkylaryl, where C1-C 10 Alkyl, C1-C 10 The article of any of the preceding clauses, wherein each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl.

[0233] Article 9. In the above formula, R A is -OC1~C 10 An article according to any of the preceding clauses, which is alkyl.

[0234] Article 10. In the above formula, R B is C6~C 20 An article according to any of the preceding clauses, which is alkyl.

[0235] Article 11. In the above formula, R B is C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 are independently deuterium or -C1 to -C 10 Alkyl-O-C1~C 10 An article according to any of the preceding clauses, which is alkyl.

[0236] Article 12. 10. The article of any preceding clause, wherein the alkyl silane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecylate)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; (phosphoundecyl)(triethoxy)silane.

[0237] Article 13. 10. The article of any preceding clause, wherein the alkylsilane is 11-chloroundecyltriethoxysilane.

[0238] Article 14. The fingerprint-invisible coating further comprises a crosslinked silane selected from the group consisting of the following formulas (I) to (IV):

[0239] (I)(SiX n )-Y 1 ,

[0240] (II)(SiX n )-Y 2 -(SiX n ),

[0241] (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and

[0242] (IV)(SiX n )-(SiX n )-Y 4 -(SiX n )-(SiX n )

[0243] During the ceremony:

[0244] Y 1 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (I) is 1 bonded to the same or different carbons in

[0245] Y 2 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (II) is 2 bonded to the same or different carbons in

[0246] Y 3 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (III) is 3 bonded to the same or different carbons in

[0247] Y 4 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (IV) is 4 bonded to the same or different carbons in

[0248] each X is independently a monovalent leaving group selected from halogen, (C1-C6)alkoxy, (C2-C6)carboxy, (C1-C6)oximo, (C1-C6)arylalkoxy; and

[0249] 10. The article of any of the preceding clauses, wherein n is an integer between 1 and 3, inclusive.

[0250] Article 15. A fingerprint-invisible composition comprising:

[0251] a solvent;

[0252] and a non-fluorinated alkylsilane hydrolysate polymer having a weight average molecular weight of less than 100,000 Da.

[0253] Article 16. 16. The fingerprint-invisible composition of clause 15, wherein the non-fluorinated alkylsilane hydrolysate polymer is present in the solvent at a concentration of at least 0.01 mg / L and less than 100 g / L.

[0254] Article 17. 10. The fingerprint-invisible composition of claim 1, wherein the solvent comprises water, alcohol, or a mixture thereof.

[0255] Article 18. The alcohol is a C1 to C 10 The fingerprint-invisible composition of any of the preceding clauses, wherein the compound is alkyl-OH.

[0256] Article 19. 10. The fingerprint-making composition of claim 1, wherein the fingerprint-making composition is acid-free.

[0257] Article 20. The non-fluorinated alkylsilane hydrolyzate polymer has the following structural formula: (R A )3SiR B and the alkylsilane is formed from an alkylsilane having the formula:

[0258] Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl;

[0259] Each R B is C1~C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 is alkynyl;

[0260] -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, -OC 10 Alkynyl, C1-C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, C(O)OR 1, -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and

[0261] Each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, or -C1-C 10 Alkyl-O-C1~C 10 alkyl;

[0262] C1~C 10 Alkylaryl-O-C1~C 10 alkylaryl, where C1-C 10 Alkyl, C1-C 10 The fingerprint-invisible composition of any of the preceding clauses, wherein each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl.

[0263] Article 21. In the above formula, R A is -OC1~C 10 The fingerprint-invisible composition of any preceding clause, wherein the alkyl is alkyl.

[0264] Article 22. In the above formula, R B C6~C 20 The fingerprint-invisible composition of any preceding clause, wherein the alkyl is alkyl.

[0265] Article 23. In the above formula, R B C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 are independently deuterium or -C1 to -C 10 Alkyl-O-C1~C 10 The fingerprint-invisible composition of any preceding clause, wherein the alkyl is alkyl.

[0266] Article 24. 11-(2-methoxyethoxy)undecyltrimethoxysilane; (aminoundecyl)(triethoxy)silane; (aminoundecyl)(trimethoxy)silane; (hydroxydecyl)(triethoxy)silane; (hydroxydecyl)(trimethoxy)silane; (undecylated)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; (phosphoundecyl)(triethoxy)silane.

[0267] Article 25. 10. The fingerprint-invisible composition of claim 1, wherein the alkylsilane is 11-chloroundecyltriethoxysilane.

[0268] Article 26. The fingerprint-invisible coating further comprises a crosslinked silane selected from the group consisting of the following formulas (I) to (IV):

[0269] (I)(SiX n )-Y 1 ,

[0270] (II)(SiX n )-Y 2 -(SiX n ),

[0271] (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and

[0272] (IV)(SiX n )-(SiX n )-Y 4 -(SiX n )-(SiX n )

[0273] During the ceremony:

[0274] Y 1 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (I) is 1 bonded to the same or different carbons in

[0275] Y 2 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (II) is 2 bonded to the same or different carbons in

[0276] Y 3 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (III) is3 bonded to the same or different carbons in

[0277] Y 4 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (IV) is 4 bonded to the same or different carbons in

[0278] each X is independently a monovalent leaving group selected from halogen, (C1-C6)alkoxy, (C2-C6)carboxy, (C1-C6)oximo, (C1-C6)arylalkoxy; and

[0279] The fingerprint-invisible composition according to any of the preceding clauses, wherein n is an integer between 1 and 3.

[0280] Article 27. 10. The fingerprint-invisible composition of claim 1, wherein the non-fluorinated alkylsilane hydrolysate polymer has a weight average molecular weight of 300 Da or more.

[0281] Article 28. 1. A method for forming a fingerprint-invisible composition, comprising:

[0282] polymerizing an alkylsilane in a first solvent comprising water and an alcohol to form a non-fluorinated alkylsilane hydrolyzate;

[0283] dissolving the non-fluorinated alkylsilane hydrolyzate in a second solvent to a concentration of at least 0.01 mg / L and less than 100 g / L.

[0284] Article 29. 29. The method of claim 28, wherein the ratio of water to alcohol in the first solvent is from 1:1000 to 1000:1.

[0285] Article 30. The method of any preceding clause, wherein the polymerizing to form the hydrolysate is carried out at a temperature of about -10°C to reflux of the first solvent.

[0286] Article 31. The alkylsilane has the following structural formula: (R A )3SiR B and

[0287] Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl;

[0288] Each R B is C1~C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 is alkynyl;

[0289] -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, -OC 10 Alkynyl, C1-C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, C(O)OR 1, -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and

[0290] Each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, or -C1-C 10 Alkyl-O-C1~C 10 alkyl;

[0291] C1~C 10 Alkylaryl-O-C1~C 10 alkylaryl, where C1-C 10 Alkyl, C1-C 10 The method of any of the preceding clauses, wherein each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl.

[0292] Article 32. In the above formula, R A The method of any of the preceding clauses, wherein is -OC1-C6 alkyl.

[0293] Article 33. In the above formula, R B C6~C 20 The method of any of the preceding clauses, wherein the alkyl group is alkyl.

[0294] Article 34. In the above formula, R B C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 is independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl.

[0295] Article 35. 10. The method of any preceding clause, wherein the alkylsilane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecylate)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; (phosphoundecyl)(triethoxy)silane.

[0296] Article 36. The method of any of the preceding clauses, wherein the alkylsilane comprises 11-chloroundecyltriethoxysilane.

[0297] Article 37. 10. The method of any of the preceding clauses, wherein the ratio of water to alcohol present in the first solvent is between 1:1000 and 1000:1.

[0298] Article 38. The method of any of the preceding clauses, wherein the alcohol comprises ethanol.

[0299] Article 39. 10. The method of any of the preceding clauses, wherein the first solvent has a pH between 0 and 14.

[0300] Article 40. 10. The method of any of the preceding clauses, wherein the first solvent has a pH between 6 and 8.

[0301] Article 41. The method of any of the preceding clauses, wherein the second solvent comprises water, an alcohol, or a mixture thereof.

[0302] Article 42. The method further comprises polymerizing the alkylsilane in the presence of a bridging silane, the bridging silane being selected from the group consisting of formulas (I) to (IV):

[0303] (I)(SiX n )-Y 1 ,

[0304] (II)(SiX n )-Y 2 -(SiX n ),

[0305] (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and

[0306] (IV)(SiX n )-(SiX n )-Y 4 -(SiX n)-(SiX n )

[0307] During the ceremony:

[0308] Y 1 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (I) is 1 bonded to the same or different carbons in

[0309] Y 2 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (II) is 2 bonded to the same or different carbons in

[0310] Y 3 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (III) is 3 bonded to the same or different carbons in

[0311] Y 4 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (IV) is 4 bonded to the same or different carbons in

[0312] each X is independently a monovalent leaving group selected from halogen, (C1-C6)alkoxy, (C2-C6)carboxy, (C1-C6)oximo, (C1-C6)arylalkoxy; and

[0313] 10. The method of any of the preceding clauses, wherein n is an integer between 1 and 3, inclusive.

[0314] Article 43. 10. The method of any preceding clause, wherein the polymerizing to form the hydrolysate is carried out for at least 0.1 hours and up to 72 hours.

[0315] Article 44. The method of any of the preceding clauses, wherein the method further comprises purifying the polymerized non-fluorinated alkylsilane hydrolyzate.

[0316] Article 45. 1. A method for forming a fingerprint-invisible surface, comprising:

[0317] On the surface of the substrate,

[0318] A solvent;

[0319] a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da and at least 300 Da; and depositing a formulation comprising:

[0320] and curing the formulation to form the fingerprint-invisible surface.

[0321] Article 46. 46. ​​The method of claim 45, wherein the depositing step comprises spraying, dipping, wiping, chemical vapor deposition (CVD), or physical vapor deposition (PVD).

[0322] Article 47. 10. The method of any of the preceding clauses, wherein the solvent comprises an alcohol.

[0323] Article 48. 48. The method of claim 47, wherein the alcohol is C1-C6 alkyl-OH.

[0324] Article 49. 10. The method of any of the preceding clauses, wherein the substrate comprises a material selected from the group consisting of glass, glass ceramic, wood, metal, metal oxide, or polymer.

[0325] Article 50. 10. The method of any preceding clause, wherein the curing to form the fingerprint-imperceptible surface comprises heating the formulation to a temperature of at least 20°C and not more than 250°C.

[0326] Article 51. 10. The method of claim 1, wherein the curing step to form the fingerprint-invisible surface is carried out for a period of at least 0.1 hours and not more than 48 hours.

[0327] Article 52. 10. The method of any preceding clause, wherein the depositing step includes forming a layer comprising the non-fluorinated alkylsilane hydrolyzate polymer having a thickness of at least 0.1 nm and not more than 300 nm.

[0328] Article 53. The method of any of the preceding clauses, wherein the formulation comprises the non-fluorinated alkylsilane hydrolysate polymer dissolved in the solvent at a concentration of 0.01 mg / L to 100 g / L.

[0329] Article 54. 10. The method of any preceding clause, wherein after curing, the fingerprint-non-visible surface has an initial contact angle using diiodomethane of less than about 45° and an initial water contact angle of greater than about 65°.

[0330] Article 55. 10. The method of any preceding clause, wherein after curing, the fingerprint-invisible coating comprises a surface having an initial contact angle using diiodomethane of less than about 50° and / or an initial water contact angle of more than about 65°.

[0331] Article 56. 10. The method of any preceding clause, wherein after curing, the fingerprint invisible coating has a coefficient of friction of less than about 0.15.

[0332] Article 57. 10. The method of any of the preceding clauses, wherein after curing, the fingerprint-invisible coating is capable of maintaining a water contact angle of at least 50 degrees after 1500 cycles of eraser abrasion.

[0333] Article 58. The non-fluorinated alkylsilane hydrolyzate polymer has the following structural formula: (R A )3SiR B and the alkylsilane is formed from an alkylsilane having the formula:

[0334] Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl;

[0335] Each R B is C1~C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 is alkynyl;

[0336] -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, -OC 10 Alkynyl, C1-C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 Each hydrogen atom in an alkynyl may independently be optionally selected from deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, C(O)OR 1, -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and

[0337] Each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, or -C1-C 10 Alkyl-O-C1~C 10 alkyl;

[0338] C1~C 10 Alkylaryl-O-C1~C 10 alkylaryl, where C1-C 10 Alkyl, C1-C 10 The method of any of the preceding clauses, wherein each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl.

[0339] Article 59. In the above formula, R A is -OC1~C 10 The method of any of the preceding clauses, wherein the alkyl group is alkyl.

[0340] Article 60. In the above formula, R B is C6~C 20 The method of any of the preceding clauses, wherein the alkyl group is alkyl.

[0341] Article 61. In the above formula, R B is C6~C 20 Alkyl, C6-C 20 Each hydrogen atom in an alkyl may be independently selected from halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, -PO3H2, where R 1 is independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl.

[0342] Article 62. 10. The method of any preceding clause, wherein the alkylsilane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecylate)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; (phosphoundecyl)(triethoxy)silane.

[0343] Article 63. 10. The method of any of the preceding clauses, wherein the alkylsilane is 11-chloroundecyltriethoxysilane.

[0344] Article 64. The formulation further comprises a crosslinked silane selected from the group consisting of formulas (I)-(IV):

[0345] (I)(SiX n )-Y 1 ,

[0346] (II)(SiX n )-Y 2 -(SiX n ),

[0347] (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and

[0348] (IV)(SiX n )-(SiX n )-Y 4 -(SiX n )-(SiX n )

[0349] During the ceremony:

[0350] Y 1 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (I) is 1 bonded to the same or different carbons in

[0351] Y 2 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (II) is 2 bonded to the same or different carbons in

[0352] Y 3 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (III) is 3 bonded to the same or different carbons in

[0353] Y 4 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, alkylaryl, and each silicon atom in formula (IV) is 4 bonded to the same or different carbons in

[0354] each X is independently a monovalent leaving group selected from halogen, (C1-C6)alkoxy, (C2-C6)carboxy, (C1-C6)oximo, (C1-C6)arylalkoxy; and

[0355] 10. The method of any of the preceding clauses, wherein n is an integer between 1 and 3, inclusive.

[0356] Article 65. 10. The method of any of the preceding clauses, wherein the formulation is acid-free.

[0357] Article 66. 10. The method of any of the preceding clauses, wherein the method further comprises activating the surface of the substrate by exposing the surface to a plasma of at least one gas selected from the group consisting of an inert gas, N2, O2, and a mixture of at least two of the foregoing gases.

[0358] Article 67. 10. The article, composition, or method of any preceding clause, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises functional groups selected from the group consisting of hydroxy, carboxy, amino, halo, and combinations thereof. Further non-limiting embodiments are given below. Article A-1. An article, a substrate comprising glass, glass ceramic, wood, metal, metal oxide, or polymer; a fingerprint-invisible coating laminated to the substrate; The fingerprint-invisible coating comprises a solvent and a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da; The non-fluorinated alkylsilane hydrolyzate polymer is (i) a structure of the following formula: (R A )3SiR B and an alkylsilane having the formula During the ceremony: Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl; R B is C6~C 20 is alkyl; (ii) a crosslinked silane selected from the group consisting of formulas (II) to (IV): (II)(SiX n )-Y 2 -(SiX n ), (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and (IV)(SiX n )-(SiX n )-Y 4 -(SiX n )-(SiX n ) During the ceremony: Y 2 (C2~C 30 ) a divalent group formed by removing one hydrogen atom from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl, and each silicon atom in formula (II) is Y 2 bonded to the same or different carbon atoms in Y 3 (C2~C 30) a trivalent group formed by removing two hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl, and each silicon atom in formula (III) is Y 3 bonded to the same or different carbon atoms in Y 4 (C2~C 30 ) a tetravalent group formed by removing three hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl, and each silicon in formula (IV) is Y 4 bonded to the same or different carbon atoms in each X is independently (C1-C6)alkoxy; and Each n is 3, The article, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises a halogen-substituted alkyl, with the proviso that the halogen of the halogen-substituted alkyl is not fluorine. Article A-2. The article of clause A-1, wherein the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 50° and / or an initial water contact angle of more than 65°. Article A-3. The article of clause A-1, wherein the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 45° and / or an initial water contact angle of more than 70°. Article A-4. The article of any one of clauses A-1 to A-3, wherein the fingerprint-invisible coating has a thickness in the range of 0.1 nm to 1000 nm. Article A-5. In the above formula, R A is -OC1~C 10 The article of any one of clauses A-1 to A-4, wherein the alkyl is alkyl. Article A-6. Each R A are independently deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, C(O)OR 1, -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and Each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, -C1-C 10 Alkyl-O-C1~C 10 Alkyl, or C1-C 10 Alkylaryl-O-C1~C 10 alkylaryl, where C1-C 10 Alkyl or C1-C 10 The article of any one of clauses A-1 to A-5, wherein each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl. Article A-7. In the above formula, R B is halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, or -PO3H2, where R 1 are independently deuterium or -C1 to -C 10Alkyl-O-C1~C 10 The article of any one of clauses A-1 to A-6, wherein the alkyl is alkyl. Article A-8. The article of any one of clauses A-1-7, wherein the alkyl silane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecyl)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; and (phosphoundecyl)(triethoxy)silane. Article A-9. The article of any one of clauses A-1 to A-8, wherein the alkylsilane is 11-chloroundecyltriethoxysilane. Article A-10. The article of any one of clauses A-1 to A-9, wherein the crosslinked silane is a BIS silane of formula (II) or a TRIS silane of formula (III). Article A-11. The article of any one of clauses A-1-10, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises functional groups selected from the group consisting of hydroxy, carboxy, amino, halo, and combinations thereof. Article A-12. 1. A method for forming a fingerprint-invisible coating on a surface of a substrate, the method comprising: On the surface of the substrate, A solvent; a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da and at least 300 Da; and depositing a fingerprint-invisible coating formulation comprising: and curing the formulation to form the fingerprint-invisible coating. The non-fluorinated alkylsilane hydrolyzate polymer is (i) a structure of the following formula: (R A )3SiR B and an alkylsilane having the formula Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl; R B is C1~C 20 Alkyl, C6-C 20 Alkylaryl, C2-C 20 Alkenyl, or C2-C 20 is alkynyl; (ii) a crosslinked silane selected from the group consisting of formulas (I) to (IV): (I)(SiX n )-Y 1 , (II)(SiX n )-Y 2 -(SiX n ), (III)(SiX n )-Y 3 -(SiX n )-(SiX n ), and (IV)(SiX n )-(SiX n )-Y 4 -(SiX n )-(SiX n ) During the ceremony: Y 1 (C2~C 30 ) linear, branched or cycloalkyl, arylalkyl, or alkylaryl, and each silicon in formula (I) is Y 1 bonded to the same or different carbon atoms in Y 2 (C2~C30 ) a divalent group formed by removing one hydrogen atom from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl, and each silicon atom in formula (II) is Y 2 bonded to the same or different carbon atoms in Y 3 (C2~C 30 ) a trivalent group formed by removing two hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl, and each silicon atom in formula (III) is Y 3 bonded to the same or different carbon atoms in Y 4 (C2~C 30 ) a tetravalent group formed by removing three hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl, and each silicon in formula (IV) is Y 4 bonded to the same or different carbon atoms in each X is independently (C1-C6)alkoxy; and The method wherein n is 3. Article A-13. The method of clause A-12, wherein the solvent comprises an alcohol. Article A-14. The method of clause A-12 or 13, wherein the substrate comprises a material selected from the group consisting of glass, glass ceramic, wood, metal, metal oxide, or polymer. Article A-15. The method of any one of clauses A-12 to A-14, wherein the step of curing to form the fingerprint-invisible coating includes heating the formulation to a temperature of at least 20°C and not more than 250°C. Article A-16. The method of any one of clauses A-12 to A-15, wherein the step of curing to form the fingerprint-invisible coating is carried out for 0.1 hours or more and 48 hours or less. Article A-17. The method of any one of clauses A-12 to A-16, wherein the laminating step includes forming a layer containing the non-fluorinated alkylsilane hydrolyzate polymer having a thickness of 0.1 nm or more and 300 nm or less. Article A-18. The method of any one of clauses A-12 to A-17, wherein the formulation comprises the non-fluorinated alkylsilane hydrolysate polymer dissolved in the solvent at a concentration of 0.01 mg / L to 100 g / L. Article A-19. The method of any one of clauses A-12 to A-18, wherein after curing, the fingerprint invisible coating has an initial oil contact angle using diiodomethane of less than 45° and an initial water contact angle of more than 65°. Article A-20. The method of any one of clauses A-12 to A-19, wherein after curing, the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 50° and / or an initial water contact angle of more than 65°. Article A-21. In the above formula, R A is -OC1~C 10 The method according to any one of clauses A-12 to A-20, wherein the alkyl is alkyl. Article A-22. In the above formula, R B is C6~C 20 The method according to any one of clauses A-12 to A-21, wherein the alkyl is alkyl. Article A-23. Each R A are independently deuterium, halogen, -OH, -CN, -OR 1 , -CO2H, C(O)OR 1, -C(O)NH2, -C(O)NH(C1-C6 alkyl), -C(O)N(C1-C6 alkyl)2, SC1-C6 alkyl, S(O)C1-C6 alkyl, -S(O)2C1-C6 alkyl, -S(O)NH(C1-C6 alkyl), -S(O)2NH(C1-C6 alkyl), S(O)N(C1-C6 alkyl)2, -S(O)2N(C1-C6 alkyl)2, -NH2, NH(C1-C6 alkyl), -N(H)C1-C6 alkyl-NH2, -N(H)C1-C6 alkyl-Si(-OC1-C6 alkyl)3, -N(R 1 )C1-C6 alkyl-N(R 1 )C1-C6 alkyl-Si(—O—C1-C6 alkyl)3-N(H)C1-C6 alkyl-N(H)C1-C6 alkyl-NH2, —P(C1-C6 alkyl)2, —P(O)(C1-C6 alkyl)2, —PO3H2, or —Si(—O—C1-C6 alkyl)3; and Each R 1 are independently deuterium, C1 to C 10 Alkyl, C1-C 10 Alkylaryl, C2-C 10 Alkenyl, C2-C 10 Alkynyl, C3-C6 cycloalkyl, C3-C6 cycloalkylaryl, -C1-C 10 Alkyl-O-C1~C 10 Alkyl; or C1-C 10 Alkylaryl-O-C1~C 10 alkylaryl, where C1-C 10 Alkyl or C1-C 10 The method according to any one of clauses A-12 to A-22, wherein each hydrogen atom in the alkylaryl is optionally replaced with a hydroxyl. Article A-24. In the above formula, R B is halogen, -OH, -CN, -OR 1 , -CO2H, -NH2, NH(C1-C6 alkyl), -N(C1-C6 alkyl)2, -P(C1-C6 alkyl)2, -P(O)(C1-C6 alkyl)2, or -PO3H2, where R 1is independently deuterium or -C1-C6 alkyl-O-C1-C6 alkyl. Article A-25. The method of any one of clauses A-12 to A-24, wherein the alkylsilane is selected from the group consisting of (chloroundecyl)(triethoxy)silane, (chloroundecyl)(trimethoxy)silane, (chlorohexyl)(triethoxy)silane, (chlorohexyl)(trimethoxy)silane, 11-(2-methoxyethoxy)undecyltrimethoxysilane, (aminoundecyl)(triethoxy)silane, (aminoundecyl)(trimethoxy)silane, (hydroxydecyl)(triethoxy)silane, (hydroxydecyl)(trimethoxy)silane; (undecyl)(triethoxy)silane; (hydroxyundecyl)(triethoxy)silane; (hydroxyheptyl)(triethoxy)silane; and (phosphoundecyl)(triethoxy)silane. Article A-26. The method according to any one of clauses A-12 to A-25, wherein the alkylsilane is 11-chloroundecyltriethoxysilane. Article A-27. The method according to any one of clauses A-12 to A-26, wherein the crosslinked silane is a BIS silane of formula (II) or a TRIS silane of formula (III). Article A-28. The method of any one of clauses A-12 to A-27, wherein the formulation is acid-free. Article A-29. The method of any one of clauses A-12 to A-28, wherein the method further comprises a step of activating the surface of the substrate by exposing the surface to a plasma of at least one gas selected from the group consisting of an inert gas, N2, O2, and a mixture of at least two of the foregoing gases. Article A-30. The method of any one of clauses A-12 to A-29, wherein the non-fluorinated alkylsilane hydrolysate polymer comprises a functional group selected from the group consisting of hydroxy, carboxy, amino, halo, and combinations thereof. Article A-31. An article, a substrate comprising glass, glass ceramic, wood, metal, metal oxide, or polymer; a fingerprint-invisible coating laminated to the substrate; the fingerprint-invisible coating comprises a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da; The non-fluorinated alkylsilane hydrolyzate polymer is (i) a structure of the following formula: (R A )3SiR B and an alkylsilane having the formula During the ceremony: Each R A are independent, -OC1~C 10 Alkyl, -OC6~C 10 Alkylaryl, -OC2~C 10 Alkenyl, or -OC 10 is alkynyl; R B is C6~C 20 is alkyl; (ii) a crosslinked silane; The article, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises a halogen-substituted alkyl, with the proviso that the halogen of the halogen-substituted alkyl is not fluorine.

[0359] Example

[0360] The following examples are set forth for illustrative purposes only, and the parts and percentages set forth in such examples are by weight unless otherwise specified.

[0361] Example 1 General Procedure 10 g of 11-chloroundecyltriethoxysilane was dissolved in 90 g of dichloromethane:isopropanol (8:1). 1 mL of 3.5% HNO3 aqueous solution was added to the reaction mixture, which was then stirred for up to 2 hours. Samples were taken at various times, including 30 minutes, 1 hour, and 2 hours. The collected samples were washed with water and dried over Na2SO4. The solvent was removed using a rotary evaporator. 0.1 g of the resulting oil was dissolved in 25 mL of isopropanol and sprayed onto glass. After keeping the coated glass in an oven at 120 °C for 15 minutes, the contact angles of diiodomethane and water were measured, and the Delta E and abrasion resistance were determined.

[0362] Example 2 synthesis 10 g of 11-chloroundecyltriethoxysilane was dissolved in 90 g of dichloromethane:isopropanol (8:1). 1 mL of 3.5% aqueous HNO3 was added to the reaction mixture, and the reaction was stirred. After stirring for 30 minutes, the reaction was quenched by washing with water. The organic phase was separated, dried over Na2SO4, and filtered. The filtrate was evaporated using a rotary evaporator. The resulting oil was collected for the next step and used to prepare the coating formulation.

[0363] Example 3 Coating formulations A formulation for coating was prepared by dissolving the hydrolysate from Example 2 in ethanol to a concentration of about 2.75 g / l of ethanol.

[0364] Example 4 Abrasion resistance

[0365] A low molecular weight alkylsilane hydrolyzate was prepared according to Example 1. The reaction time was 1 hour. A formulation for a fingerprint-resistant coating was prepared according to Example 3 and sprayed onto Gorilla Glass. The coating was cured at 125°C for 20 minutes and then at room temperature overnight. Abrasion resistance was measured according to ASTM D4060. A CS-10 hardness abrasive disc was used to ablate the specimens at a 1.5 cm 2The tests were carried out under a load of 250 g over an area of ​​100 mm, using a translational speed of 50 cycles / min and a rotational speed of 6 rpm. The initial contact angles with water and oil (diiodomethane) were measured. The tests were carried out for 1,000 or 2,000 cycles. After the cycles, the contact angle with water was measured.

[0366] [Table 1]

[0367] Example 5 Friction coefficient The formulation according to Example 3 was sprayed onto Gorilla Glass. The coated glass was cured at 125°C for 1 hour. The coefficient of friction was measured using a Labthink FPT-F1 Friction / Peel Tester. The resulting value was 0.108.

[0368] Example 6 Synthesis of PDMS-TEOS Monovinyl-terminated PDMS (5k) (10 g, 0.002 mol, 1 eq.; available from Gelest) and triethoxysilane (0.5 g, 0.003 mol, 1.5 eq.) were dissolved in 5 mL of anhydrous toluene and purged under Ar for 30 minutes. 0.1 mL of Pt(Dvs) (available from Sigma-Aldrich) was added to the reaction mixture, which was then heated to 90°C. The reaction mixture was stirred at 90°C for approximately 60 hours. After cooling to room temperature, the reaction mixture was directly filtered through Celite. Yield: 7.9 g.

[0369] Example 7 PDMS-TEOS hydrolysate 5 g of 11-chloroundecyltriethoxysilane and 0.5 g of PDMS-TEOS were dissolved in 55 g of dichloromethane:isopropanol (10:1). 0.5 mL of 7% aqueous HNO3 was added to the reaction mixture and stirred. After 15 minutes, 30 minutes, and 1 hour, samples were taken from the reaction mixture and washed with water for post-treatment. The organic phase was separated, dried over Na2SO4, and filtered. The filtrate was evaporated using a rotary evaporator. A fingerprint-invisible coating formulation was prepared by dissolving oil in ethanol to a concentration of approximately 2.5 g / L.

[0370] Example 8 Abrasion resistance The formulation according to Example 7 was sprayed onto Gorilla Glass. The coated glass was cured at 125°C for 20 minutes. The spraying and baking steps were repeated three times for a total of four layers. The coated glass was allowed to cure overnight at room temperature. The initial water and oil (CH2I2) contact angles were measured. The coated glass was then abraded according to Example 4. The results are shown in Table 2.

[0371] [Table 2]

[0372] Example 9 Abrasion resistance The formulation according to Example 7 was sprayed onto Gorilla Glass. The coated glass was cured at 125°C for 20 minutes. The spraying and baking steps were repeated three times to achieve four layers. The coated glass was allowed to cure overnight at room temperature. The initial water and oil (CH2I2) contact angles were measured. The coated glass was then abraded according to Example 4. The results are shown in Table 3.

[0373] [Table 3]

[0374] Example 10 Abrasion resistance The formulation according to Example 7 was sprayed onto Gorilla Glass. The coated glass was cured at 125°C for 20 minutes. The spraying and baking steps were repeated once for a total of two layers. The coated glass was cured at room temperature for 30 minutes. The initial water and oil (CH2I2) contact angles were measured. The coated glass was then abraded according to Example 4. The results are shown in Table 4.

[0375] [Table 4]

[0376] Example 11 Abrasion resistance The formulation according to Example 7 was sprayed onto Gorilla Glass. The coated glass was cured at 150°C for 1 hour. The spraying and baking steps were repeated three times for a total of four layers. The initial water and oil (CH2I2) contact angles were measured before curing. The coated glass was cured overnight at room temperature. The initial water and oil (CH2I2) contact angles were measured. The coated glass was then abraded according to Example 4. The results are shown in Table 5.

[0377] [Table 5]

[0378] Example 12 Delta E To measure fingerprint performance, the LAB value of a virgin glass sheet against a black background, ideally using black cardstock or a black OLED display, was measured. Next, the operator was asked to wipe their nose or forehead, the oiliest part of their body, two to three times using all four fingers of their dominant hand. They then immediately tapped the glass with all four fingers using moderate pressure 10 times, resulting in 40 fingerprints on the glass surface. They then measured the LAB value using a colorimeter and used these values ​​to calculate a Delta E based on the virgin glass sheet and the glass sheet with the fingerprints. The lower the Delta E, the less visible the fingerprints. Next, the operator took a piece of jeans material, ideally standardized LEVIS 401 jeans material, and wiped the glass sheet twice along the same area to remove the fingerprints. The operator then calculated the Delta E compared to the virgin glass sheet to determine the cleanability of the coating. The closer the value was to 0, the less visible the fingerprints.

[0379] Different hydrolysis reaction times (according to Example 2) were analyzed. A formulation for a fingerprint-invisible coating was prepared according to Example 3. The fingerprint-invisible coating was formed according to Example 4. The results are shown in Table 6.

[0380] [Table 6]

[0381] The following chemicals listed in Table 7 were used in the following examples.

[0382] [Table 7]

[0383] Example 13 compound 10 g of 11-chloroundecyltriethoxysilane, 70 mL of anhydrous 200-proof ethanol (ethyl alcohol (pure)), and 0.8 mL of deionized water were charged into a 100 mL round-bottom flask equipped with a reflux condenser. While mixing, the solution was heated to reflux, approximately 79 °C, and held for 20 hours. Next, the reaction mixture was rotary evaporated to full vacuum at 45-55 °C to remove the ethanol and water, yielding 8.3 g of polychloroundecylsiloxane.

[0384] Examples 14 to 16 Examples 14-16 were prepared in the same manner as Example 13, except that the amount of water added to the reactants was varied to alter the degree of hydrolysis and condensation of the polychloroundecylsiloxane formed, as shown in Table 8.

[0385] [Table 8]

[0386] The polychloroundecylsiloxanes produced from Examples 13-16 were analyzed using gel permeation chromatography (GPC), and the results are shown in Table 9. The polychloroundecylsiloxanes produced using higher water to ethoxy ratios achieve higher molecular weights and polydispersities.

[0387] [Table 9]

[0388] The polychloroundecylsiloxanes produced from Examples 13-16 were analyzed using Fourier transform infrared spectroscopy (FTIR). An overlay of the FTIRs from four examples and the starting material, 11-chloroundecyltriethoxysilane (labeled "CLAS"), is shown in Figure 1. All four samples exhibited peaks between 3200 and 3500 cm. -1 The formation of a broad stretch between 1100 and 1200 cm is indicative of the formation of hydroxyl groups. -1As the water to ethoxy ratio gradually increases, this FTIR stretch becomes increasingly broader, indicating a higher polychloroundecylsiloxane content.

[0389] The polychloroundecylsiloxanes produced in Examples 13-16 were analyzed using proton nuclear magnetic resonance spectroscopy (NMR). NMR "integral analysis" was used to determine the "extent of reaction" by comparing the "ethoxy groups" remaining after the reaction. Table 10 below shows the calculated extent of reaction for Examples 13-16. A gradual increase in the water to ethoxy ratio resulted in a gradual increase in the extent of reaction, resulting in a decrease in the amount of unreacted starting material in the final product.

[0390] [Table 10]

[0391] Example 17 coating Four of the polychloroundecylsiloxane samples from Examples 13-16 were coated on glass panels and cured. Once cured, the initial water contact angle (IWA) was measured using a water drop, and the initial diiodomethane contact angle (IDA) was measured using a goniometer. After the initial angles were measured, the coatings were linearly abraded for 1500 cycles, after which the contact angles were measured again. These same samples were abraded for an additional 1500 cycles, for a total of 3000 cycles, and the contact angles were measured again. Table 11 below shows the initial and abraded contact angles for the four coated polychloroundecylsiloxane samples.

[0392] [Table 11]

[0393] Example 18 compound 10 g of 11-chloroundecyltriethoxysilane, 0.72 g of 1,2-bis(triethoxysilyl)ethane (BIS), 70 mL of anhydrous 200-proof ethanol, and 0.88 mL of deionized water were charged into a 100 mL round-bottom flask equipped with a reflux condenser. While mixing, the solution was heated to reflux, approximately 79 °C, and held for 20 h. The reaction mixture was then rotary evaporated to full vacuum at 45-55 °C to remove the ethanol and water, yielding 8.8 g of polychloroundecylsiloxane.

[0394] Examples 19 to 21 Examples 19-21 were prepared in the same manner as Example 16, except that the amount of water added to the reaction was varied to alter the extent of hydrolysis and condensation of the polychloroundecylsiloxane formed. Table 12 provides details of these four examples. Example 21 was run at double the scale.

[0395] [Table 12]

[0396] The polychloroundecylsiloxanes produced from Examples 18-21 were analyzed using gel permeation chromatography (GPC) and the results are shown in Table 13. The polychloroundecylsiloxanes produced using a higher water to ethoxy ratio achieve higher molecular weights and polydispersities.

[0397] [Table 13]

[0398] The polychloroundecylsiloxanes produced from Examples 18-21 were analyzed using Fourier transform infrared spectroscopy (FTIR). An overlay of the FTIRs from four examples and the starting material, 11-chloroundecyltriethoxysilane (labeled "CLAS"), is shown in Figure 2. All four samples exhibited peaks between 3200 and 3500 cm. -1The formation of a broad stretch between 1100 and 1200 cm is indicative of the formation of hydroxyl groups. -1 As the water to ethoxy ratio gradually increases, this FTIR stretch becomes increasingly broader, indicating a higher polychloroundecylsiloxane content.

[0399] The polychloroundecylsiloxanes produced in Examples 18-21 were analyzed using proton nuclear magnetic resonance spectroscopy (NMR). NMR "integral analysis" was used to determine the "extent of reaction" by comparing the "ethoxy groups" remaining after the reaction. Table 14 below shows the calculated extent of reaction for Examples 18-21. A gradual increase in the water to ethoxy ratio resulted in a gradual increase in the extent of reaction, resulting in a decrease in the amount of unreacted starting material in the final product.

[0400] [Table 14]

[0401] Example 22 coating Four of the polychloroundecylsiloxane samples from Examples 18-21 were coated on glass panels and cured. Once cured, the initial water contact angle (IWA) was measured using a water drop, and the initial diiodomethane contact angle (IDA) was measured using a goniometer. After the initial angles were measured, the coatings were linearly abraded for 1500 cycles, after which the contact angles were measured again. These same samples were abraded for an additional 1500 cycles, for a total of 3,000 cycles, and the contact angles were measured again. Table 15 below shows the initial and abraded contact angles for the four coated polychloroundecylsiloxane samples.

[0402] [Table 15]

[0403] Example 23 compound 10 g of 11-chloroundecyltriethoxysilane, 1.04 g of 1,2-tris(triethoxysilyl)ethane (TRIS), 70 mL of anhydrous 200-proof ethanol, and 0.93 mL of deionized water were charged into a 100 mL round-bottom flask equipped with a reflux condenser. While mixing, the solution was heated to reflux, approximately 79 °C, and held for 20 hours. The reaction mixture was then rotary evaporated to full vacuum at 45-55 °C to remove the ethanol and water, yielding 9.2 g of polychloroundecylsiloxane.

[0404] Examples 24 to 26 Examples 24-26 were prepared in the same manner as Example 23, except that the amount of water added to the reaction was varied to alter the degree of hydrolysis and condensation of the polychloroundecylsiloxane formed. Table 16 provides details of these four examples. Example 26 was run at twice the scale.

[0405] [Table 16]

[0406] The polychloroundecylsiloxanes produced from Examples 23-26 were analyzed using gel permeation chromatography (GPC), and the results are shown in Table 17. Polychloroundecylsiloxanes produced using higher water to ethoxy ratios achieve higher molecular weights and polydispersities.

[0407] [Table 17]

[0408] The polychloroundecylsiloxanes produced from Examples 23-26 were analyzed using Fourier transform infrared spectroscopy (FTIR). An overlay of the FTIRs from four examples and the starting material, 11-chloroundecyltriethoxysilane (labeled "CLAS"), is shown in Figure 3. All four samples exhibited peaks between 3200 and 3500 cm. -1The formation of a broad stretch between 1100 and 1200 cm is indicative of the formation of hydroxyl groups. -1 As the water to ethoxy ratio gradually increases, this FTIR stretch becomes increasingly broader, indicating a higher polychloroundecylsiloxane content.

[0409] The polychloroundecylsiloxanes produced in Examples 23-26 were analyzed using proton nuclear magnetic resonance spectroscopy (NMR). NMR "integral analysis" was used to determine the "extent of reaction" by comparing the "ethoxy groups" remaining after the reaction. Table 18 below shows the calculated extent of reaction for Examples 21-24. A gradual increase in the water to ethoxy ratio resulted in a gradual increase in the extent of reaction, resulting in a decrease in the amount of unreacted starting material in the final product.

[0410] [Table 18]

[0411] Four of the polychloroundecylsiloxane samples from Examples 23-26 were coated on glass panels and cured. Once cured, the initial water contact angle (IWA) was measured using a water drop, and the initial diiodomethane contact angle (IDA) was measured using a goniometer. After measuring the initial angle, the coatings were linearly abraded for 1,500 cycles, after which the contact angle was measured again. These same samples were abraded for an additional 1,500 cycles, for a total of 3,000 cycles, and the contact angle was measured again. Table 19 below shows the initial and abraded contact angles for the four coated polychloroundecylsiloxane samples.

[0412] [Table 19]

[0413] Example 27 thermogravimetric analysis Thermogravimetric analysis (TGA) was performed on a TA Instruments Discovery Series thermogravimetric analyzer. Samples were heated in platinum pans from room temperature to 700°C at a heating rate of 20°C / min under a nitrogen purge (25 mL / min). The TGA data for 11-chloroundecyltriethoxysilane is shown in FIG.

[0414] To understand the polymerization of the formulations described herein, the water to ethoxy ratio was varied for the following reagent mixtures: pure 11-chloroundecyltriethoxysilane, 14:1 11-chloroundecyltriethoxysilane to 1,2-bis(triethoxysilyl)ethane, and 14:1 11-chloroundecyltriethoxysilane to 1,1,2-tris(triethoxysilyl)ethane. For each sample set, four experiments were performed using the following water to ethoxy ratios: 1.0:2.0, 1.0:1.0, 2.0:1.0, and 3.0:1.0. Reaction temperature, time, and pH were all controlled.

[0415] Higher molecular weights can appear in TGA as a weight loss shift to the right (higher temperature) on a graph of weight loss versus temperature, or as a peak in the weight loss of the derivative occurring at higher temperatures. In the case of siloxanes, a second weight loss step can also be observed at 500 °C, where the Si-O-Si linkages decompose. This weight loss step is particularly noticeable in the weight loss of the derivative versus temperature. Experiments using pure 11-chloroundecyltriethoxysilane with varying water to ethoxy ratios are shown in Figures 5 and 6.

[0416] The reaction parameters are held constant while increasing the amount of water equivalents present in the reaction. By incorporating more water into the reaction, more hydrolysis occurs, which can increase the concentration of silanol bonds and increase the degree of polymerization.

[0417] The TGA data show that the decomposition onset temperature increased for samples with higher water content, with a higher derivative weight loss peak observed at 500 °C. This may be due to the abundance of -Si-O-Si- bonds formed by polymerization. The thermal decomposition temperature of these bonds is approximately 500 °C.

[0418] The two samples with the highest water content showed weight loss at 100°C, which may be due to residual water remaining in the samples or additional condensation of silanol end groups. The sample with the highest water content during the reaction is the one that forms the highest concentration of Si-OH bonds.

[0419] From the TGA data, it was observed that the decomposition temperature increased for samples with a higher water content, and a higher peak weight loss of the derivative was observed at 500°C. This is due to the increased -Si-O-Si- bonds formed by polymerization. The thermal decomposition temperature of these bonds is approximately 500°C.

[0420] Interestingly, the two samples with the highest water content show significant weight loss at 100°C. This may be due to residual water remaining in the sample or additional condensation of silanol end groups. The sample with the highest water content during the reaction forms a higher concentration of Si-OH bonds.

[0421] Experiments in which the water to ethoxy ratio in a 14:1 mixture of 11-chloroundecyltriethoxysilane and 1,2-bis(triethoxysilyl)ethane (BIS) was varied are shown in Figures 7 and 8. Similar trends were observed as in the experiments with pure 11-chloroundecyltriethoxysilane, with the onset temperature of decomposition increasing (shifting to the right) and the magnitude of the weight loss peak for the derivative at 500 °C increasing with increasing water content.

[0422] Experiments in which the water to ethoxy ratio in a 14:1 mixture of 11-chloroundecyltriethoxysilane and 1,1,2-tris(triethoxysilyl)ethane (TRIS) was varied are shown in Figures 9 and 10. Similar trends were observed as in the experiments with pure 11-chloroundecyltriethoxysilane and 11-chloroundecyltriethoxysilane + BIS in a 14:1 ratio, with the onset of decomposition temperature increasing (right shift) and, to a lesser extent, the magnitude of the weight loss peak for the derivative at 500 °C increasing with increasing water content.

[0423] The decomposition temperature shift is much smaller for all 11-chloroundecyltriethoxysilane and TRIS samples compared to the previous two sample sets. This may suggest that the reaction of 11-chloroundecyltriethoxysilane, TRIS, and water may occur more quickly than with 11-chloroundecyltriethoxysilane alone or with BIS. In particular, for the reaction of 11-chloroundecyltriethoxysilane with TRIS, a significant decomposition peak is observed at 100 °C when the water-to-ethoxy ratio exceeds 2:1. This may indicate the presence of water due to impure solvent and water removal at the end of the process, or it may be due to unreacted silanol groups that continue to condense and release water into the final IFP hydrolyzate. The magnitude of the decomposition peak at 500 °C does not show a clear increasing trend compared to 11-chloroundecyltriethoxysilane alone and 11-chloroundecyltriethoxysilane with BIS. This may suggest that the water to ethoxy ratios studied may be well beyond the saturation point of the silanol / siloxane hydrolysis / condensation reaction.

[0424] From samples set up with various water-to-ethoxy ratios, TGA data suggests that increasing the amount of water to increase hydrolysis within the reaction may lead to even higher degrees of polymerization resulting from condensation.

[0425] Example 28 Gel Permeation Chromatography (GPC) The molecular weights of the IFP hydrolysates were determined using a Shimadzu Prominence-I LC-2030C Plus GPC. Figure 11 shows an overlay of the molecular weight of the 11-chloroundecyltriethoxysilane starting material with four different IFP hydrolysates. These IFP hydrolysates were made from the same 11-chloroundecyltriethoxysilane starting material, but using four different water-to-alkoxy ratios: 1:2, 1:1, 2:1, and 3:1. The results are shown in Figure 11. As the water level increases, the final molecular weight increases, as indicated by a shift in the molecular weight distribution to the right.

[0426] At water to ethoxy ratios of 3:1 or greater, over 87% of the starting material can be converted to oligomers or polymers.

[0427] While the methods, apparatus, and systems have been described in connection with specific embodiments, the embodiments herein are intended in all respects to be illustrative and not restrictive, and therefore the scope of the invention is not intended to be limited to the particular embodiments described.

[0428] Unless otherwise expressly stated, it is in no way intended that any method described herein be construed as requiring that its steps be performed in a particular order. Thus, unless a method claim actually recites the order in which its steps must be followed, or unless the claim or specification specifically states that the steps are limited to a particular order, no order is intended to be inferred in any respect.

[0429] Ranges may be expressed herein as from "about" one particular value, and / or to "about" another particular value. When such a range is expressed, another embodiment includes from the one particular value and / or to the other particular value. Similarly, when values ​​are expressed as approximations, by use of the antecedent "about," it will be understood that the particular value forms another embodiment. Furthermore, It will be understood that the endpoints of each of the ranges are significant in both respects and independently of the other endpoint.

[0430] Disclosed are components that can be used to implement the disclosed methods, apparatus, and systems. These and other components are disclosed herein, and where combinations, subsets, interactions, groups, etc. of these components are disclosed, specific reference to each of their various individual and collective combinations and permutations is not expressly disclosed, but each is specifically contemplated and described herein for all methods, apparatus, and systems. This applies to all aspects of this application, including, but not limited to, the steps of the disclosed methods. Thus, where there are a variety of additional steps that can be implemented, it is understood that each of these additional steps can be implemented in any specific embodiment or combination of embodiments of the disclosed methods.

[0431] It should further be noted that all patents, applications, and publications referenced herein are incorporated by reference in their entirety.

Claims

1. An article, a substrate comprising glass, glass ceramic, wood, metal, metal oxide, or polymer; a fingerprint-invisible coating laminated to the substrate; The fingerprint-invisible coating comprises a solvent and a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da; The non-fluorinated alkylsilane hydrolyzate polymer is (i) an alkylsilane, which is 11-chloroundecyltriethoxysilane; ； (ii) a crosslinked silane selected from the group consisting of formulas (II) to (IV): (II)(SiX ｎ )-Y ２ -(SiX ｎ )、 (III) (SiX ｎ )-Y ３ -(SiX ｎ )-(SiX ｎ ), and (IV)(SiX ｎ )-(SiX ｎ )-Y ４ -(SiX ｎ )-(SiX ｎ ) During the ceremony: Y ２ (C ２ ~C ３０ ) a divalent group formed by removing one hydrogen atom from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl; each silicon in formula (II) is Y ２ bonded to the same or different carbon atoms in Y ３ (C ２ ~C ３０ ) a trivalent group formed by removing two hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl; each silicon atom in formula (III) is Y ３ bonded to the same or different carbon atoms in Y ４ (C ２ ~C ３０ ) a tetravalent group formed by removing three hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl; each silicon in formula (IV) is Y ４ bonded to the same or different carbon atoms in Each X is independently selected from the group consisting of (C １ ~C ６ ) alkoxy, and Each n is 3; The article, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises a halogen-substituted alkyl, with the proviso that the halogen of the halogen-substituted alkyl is not fluorine.

2. 10. The article of claim 1, wherein the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 50° and / or an initial water contact angle of more than 65°.

3. 10. The article of claim 1, wherein the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 45° and / or an initial water contact angle of more than 70°.

4. The article according to any one of claims 1 to 3, wherein the fingerprint-invisible coating has a thickness in the range of 0.1 nm to 1000 nm.

5. The article of any one of claims 1 to 4, wherein the crosslinked silane is a BIS silane of formula (II) or a TRIS silane of formula (III).

6. The article of any one of claims 1 to 5, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises functional groups selected from the group consisting of hydroxy, carboxy, amino, halo, and combinations thereof.

7. 1. A method for forming a fingerprint-invisible coating on a surface of a substrate, the method comprising: On the surface of the substrate, A solvent; a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da and at least 300 Da; and depositing a fingerprint-invisible coating formulation comprising: and curing the formulation to form the fingerprint-invisible coating. The non-fluorinated alkylsilane hydrolyzate polymer is (i) an alkylsilane which is 11-chloroundecyltriethoxysilane; (ii) a crosslinked silane selected from the group consisting of formulas (I) to (IV): (I)(SiX ｎ )-Y １ 、 (II)(SiX ｎ )-Y ２ -(SiX ｎ )、 (III) (SiX ｎ )-Y ３ -(SiX ｎ )-(SiX ｎ ), and (IV)(SiX ｎ )-(SiX ｎ )-Y ４ -(SiX ｎ )-(SiX ｎ ) During the ceremony: Y １ (C ２ ~C ３０ ) linear, branched or cycloalkyl, arylalkyl, or alkylaryl, and each silicon in formula (I) is １ bonded to the same or different carbon atoms in Y ２ (C ２ ~C ３０ ) a divalent group formed by removing one hydrogen atom from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl; each silicon in formula (II) is Y ２ bonded to the same or different carbon atoms in Y ３ (C ２ ~C ３０ ) a trivalent group formed by removing two hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl; each silicon atom in formula (III) is Y ３ bonded to the same or different carbon atoms in Y ４ (C ２ ~C ３０ ) a tetravalent group formed by removing three hydrogen atoms from a linear, branched, or cycloalkyl, arylalkyl, or alkylaryl; each silicon in formula (IV) is Y ４ bonded to the same or different carbon atoms in Each X is independently selected from the group consisting of (C １ ~C ６ ) alkoxy, and The method wherein n is 3.

8. The method of claim 7 , wherein the solvent comprises an alcohol.

9. 9. The method of claim 7 or 8, wherein the substrate comprises a material selected from the group consisting of glass, glass ceramic, wood, metal, metal oxide, or polymer.

10. 10. The method of any one of claims 7 to 9, wherein the curing to form the fingerprint invisible coating comprises heating the formulation to a temperature of at least 20°C and at most 250°C.

11. The method according to any one of claims 7 to 10, wherein the step of curing to form the fingerprint invisible coating is carried out for a period of not less than 0.1 hours and not more than 48 hours.

12. 11. The method of claim 7, wherein the depositing step comprises forming a layer comprising the non-fluorinated alkylsilane hydrolyzate polymer having a thickness of 0.1 nm or more and 300 nm or less.

13. The method of any one of claims 7 to 12, wherein the formulation comprises the non-fluorinated alkylsilane hydrolysate polymer dissolved in the solvent at a concentration of 0.01 mg / L to 100 g / L.

14. 14. The method of any one of claims 7 to 13, wherein after curing, the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 45° and an initial water contact angle of more than 65°.

15. 15. The method according to any one of claims 7 to 14, wherein after curing, the fingerprint-invisible coating has an initial oil contact angle using diiodomethane of less than 50° and / or an initial water contact angle of more than 65°.

16. 16. The method of any one of claims 7 to 15, wherein the crosslinked silane is a BIS silane of formula (II) or a TRIS silane of formula (III).

17. The method of any one of claims 7 to 16, wherein the formulation is acid-free.

18. The method further comprises adding an inert gas, N ２ , O ２ 18. The method according to any one of claims 7 to 17, comprising activating the surface of the substrate by exposing it to a plasma of at least one gas selected from the group consisting of:

19. 19. The method of any one of claims 7 to 18, wherein the non-fluorinated alkylsilane hydrolysate polymer comprises functional groups selected from the group consisting of hydroxy, carboxy, amino, halo, and combinations thereof.

20. An article, a substrate comprising glass, glass ceramic, wood, metal, metal oxide, or polymer; a fingerprint-invisible coating laminated to the substrate; the fingerprint-invisible coating comprises a non-fluorinated alkylsilane hydrolyzate polymer having a weight average molecular weight of less than 100,000 Da; The non-fluorinated alkylsilane hydrolyzate polymer is (i) an alkylsilane which is 11-chloroundecyltriethoxysilane; (ii) a crosslinked silane; The article, wherein the non-fluorinated alkylsilane hydrolyzate polymer comprises a halogen-substituted alkyl, with the proviso that the halogen of the halogen-substituted alkyl is not fluorine.

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