Gas-reactive film multilayered object and skin gas analysis method

Abstract

This gas-reactive film multilayered object comprises a base material made of a resin, and a light-emitting layer containing a gas-reactive light-emitting material. The base material has a moisture permeability of less than 7 g / m2·24 h. Preferably, the base material has an average light transmittance of at least 80% at a wavelength of 300-400 nm. The gas-reactive light-emitting material reacts with skin gas. The photoluminescent properties of the gas-reactive light-emitting material change due to reaction with a gas. Also provided is a skin gas analysis method using said gas-reactive film multilayered object.

Description

Gas-reactive film composite and skin gas analysis method

[0001] The present invention relates to a gas-reactive film composite and a method for analyzing skin gases.

[0002] It is sometimes necessary to capture trace amounts of gases emitted from the surface of an object and obtain information about the emission (e.g., the type and amount of gas emitted). For example, by capturing trace amounts of gases emitted from the surface of a living organism (e.g., the skin of humans and non-human animals) and obtaining information about the emission, information about the inside of the living organism can be obtained. Known instruments for obtaining information about such gas emission include analytical instruments equipped with a component containing a luminescent material that reacts with the gas. During analysis, such an analytical instrument is placed or attached to the surface of the object to be analyzed, maintained in this state for a certain analysis period, and then removed from the object. The analysis can then be performed by measuring the degree of luminescence from the luminescent material with a measuring device.

[0003] For example, Patent Documents 1 and 2 describe the analysis of gases emitted from living organisms using a substance that exhibits the property of emitting fluorescence in response to the gases.

[0004] As an example of an analytical instrument, Patent Document 3 discloses a chemical substance sensor that includes a functional member including a flat, disk-shaped trapping agent that captures chemical substances and a pair of porous disk-shaped members that sandwich the trapping agent, and that is housed in a case that also includes a mechanism such as a magnet.As another example of an analytical instrument, Patent Document 4 discloses a skin gas measuring device that includes a disk-shaped detecting agent and a container that houses the detecting agent.

[0005] International Publication No. 2023 / 008399 International Publication No. 2019 / 103130 (Corresponding Publication: U.S. Patent Application Publication No. 2021 / 361224) International Publication No. 2022 / 004685 (Corresponding Publication: U.S. Patent Application Publication No. 2023 / 117850) JP 2018-141711 A

[0006] Depending on the type of analysis, it may be necessary to suppress deterioration of the luminescent material due to intrusion of moisture or the like from the outside air from the side of the analytical instrument opposite the object to be analyzed while the analytical instrument is placed on the surface of the object to be analyzed. In such cases, the analytical instruments disclosed in Patent Documents 3 and 4 cannot sufficiently suppress such undesired deterioration.

[0007] In another aspect, the layer that holds the luminescent material may be required to retain a certain amount of moisture to maintain its performance while the analytical instrument is placed on the surface of an object to be analyzed. In such cases, the analytical instruments disclosed in Patent Documents 3 and 4 are unable to sufficiently achieve such moisture retention because the moisture in the layer easily evaporates outside the instrument.

[0008] Furthermore, when an analytical instrument is attached to the surface of a flexible object whose shape changes, such as the surface of the skin of a living body, the analytical instrument is required to have flexibility to follow the shape of the surface. With the analytical instruments disclosed in Patent Documents 3 and 4, it is difficult to obtain such flexibility, and the ease of handling is insufficient.

[0009] Furthermore, analytical instruments often need to be stored for a long period of time between their manufacture and use. In the analytical instruments disclosed in Patent Documents 3 and 4, the gas-sensitive luminescent material is not protected, and therefore it becomes necessary to enclose the instrument in an additional protective member or the like in order to store it for a long period of time prior to use.

[0010] Therefore, an object of the present invention is to provide an instrument for analyzing trace amounts of gas emitted from the surface of an object to be analyzed, which is easy to store, can suppress deterioration while placed on the surface of the object to be analyzed, and is easy to handle, and to provide an analytical method that can easily accomplish such analysis.

[0011] The present inventors have conducted research to solve the above-mentioned problems. As a result, the present inventors have found that the above-mentioned problems can be solved by constructing a gas-reactive film multilayer structure as an analytical instrument, which structure includes a specific substrate and a luminescent layer containing a gas-reactive luminescent material. In particular, since deterioration of the luminescent layer is often largely related to changes in the moisture content in the luminescent layer, the inventors have conceived that the above-mentioned problems can be effectively solved by using a substrate with a specific low moisture permeability. The present invention was made based on the above findings. Specifically, the present invention includes the following:

[0012] (1) A gas-reactive film composite comprising a base material made of a resin and a light-emitting layer containing a gas-reactive light-emitting material, the base material having a moisture permeability of less than 7 g / m2·24 h. (2) The gas-reactive film composite according to (1), wherein the base material has an average light transmittance of 80% or more at wavelengths of 300 to 400 nm. (3) The gas-reactive film composite according to (1) or (2), wherein the base material has an average light transmittance of 85% or more at wavelengths of 400 to 750 nm. (4) The gas-reactive film composite according to any one of (1) to (3), wherein the gas-reactive light-emitting material is a material that reacts with skin gas. (5) The gas-reactive film composite according to any one of (1) to (4), wherein the gas-reactive light-emitting material is a material whose photoluminescent properties change upon reaction with gas. (6) The gas-reactive film composite according to any one of (1) to (5), wherein the resin contains an alicyclic structure-containing polymer. (7) The gas-reactive film composite according to (6), wherein the alicyclic structure-containing polymer is a norbornene-based polymer, and the norbornene-based polymer comprises at least one selected from the group consisting of a hydrogenated ring-opening polymer of a monomer having a norbornene structure, an addition copolymer of a monomer having a norbornene structure and an α-olefin, and a hydrogenated product thereof. (8) The gas-reactive film composite according to (6), wherein the alicyclic structure-containing polymer is a hydrogenated block copolymer [E], and the hydrogenated block copolymer [E] is a hydrogenated block copolymer obtained by hydrogenating a block copolymer [D] consisting of: a polymer block [A] mainly composed of a repeating unit [I] derived from an aromatic vinyl compound; and a polymer block [B] mainly composed of a repeating unit [I] derived from an aromatic vinyl compound and a repeating unit [II] derived from a linear conjugated diene compound, or a polymer block [C] mainly composed of a repeating unit [II] derived from a linear conjugated diene compound. (9) The gas reactive film composite according to any one of (1) to (8), further comprising a protective layer provided on the substrate opposite the light emitting layer. (10) The gas reactive film composite according to any one of (1) to (9), further comprising a peelable sealing layer provided on the surface of the light emitting layer opposite the substrate.(11) A skin gas analysis method comprising: Step 1: preparing the gas-reactive film composite according to any one of (1) to (10); Step 2: placing the gas-reactive film composite on the skin of a subject to cause a skin gas to react with the gas-reactive luminescent material in the gas-reactive film composite; and Step 4: irradiating the gas-reactive luminescent material with excitation light and detecting fluorescence or phosphorescence emitted from the gas-reactive luminescent material. (12) The skin gas analysis method according to (11), further comprising Step 3: sealing the gas-reactive luminescent material to which the skin gas has reacted with the skin gas, with a sealing substrate, after Step 2 and before Step 4. (13) The skin gas analysis method according to (12), wherein the sealing substrate is made of a resin containing an alicyclic structure-containing polymer. (14) The skin gas analysis method according to (12), wherein the sealing substrate is a black film. (15) The skin gas analysis method according to (12), wherein the sealing substrate is a reflector.

[0013] According to the present invention, there is provided a gas-reactive film composite for analyzing trace amounts of gas emitted from the surface of an object to be analyzed, which is easy to store, can suppress deterioration while placed on the surface of the object to be analyzed, and is easy to handle; and an analytical method that can easily achieve such analysis.

[0014] FIG. 1 is a longitudinal sectional view schematically showing one example of a gas reactive film laminate of the present invention. FIG. 2 is a longitudinal sectional view schematically showing another example of a gas reactive film laminate of the present invention. FIG. 3 is a longitudinal sectional view schematically showing yet another example of a gas reactive film laminate of the present invention. FIG. 4 is a longitudinal sectional view schematically showing yet another example of a gas reactive film laminate of the present invention. FIG. 5 is a longitudinal sectional view schematically showing yet another example of a gas reactive film laminate of the present invention. FIG. 6 is a longitudinal sectional view schematically showing an example of a state in which the gas reactive film laminate shown in FIG. 2 is subjected to step 2 of the analytical method of the present invention. FIG. 7 is a longitudinal sectional view schematically showing an example of a state in which the gas reactive film laminate shown in FIG. 6 is subjected to step 3 of the analytical method of the present invention. FIG. 8 is a longitudinal sectional view schematically showing an example of a state in which the gas reactive film laminate shown in FIG. 4 is subjected to step 2 of the analytical method of the present invention. FIG. 9 is a longitudinal sectional view schematically showing an example of a state in which the gas reactive film laminate shown in FIG. 8 is subjected to step 3 of the analytical method of the present invention.

[0015] The present invention will be described below with reference to embodiments and examples. However, the present invention is not limited to the embodiments and examples described below, and may be modified and implemented within the scope of the claims and their equivalents.

[0016] <Gas Reactive Film Multilayer> The gas reactive film multilayer of the present invention comprises a base material made of a resin and a light-emitting layer containing a gas reactive light-emitting material.

[0017] <Gas-reactive film composite: substrate> In the gas-reactive film composite of the present invention, the substrate is made of a resin. A substrate made of a resin is a solid film and may have flexibility. By including such a substrate in the gas-reactive film composite, the light-emitting layer can be well protected, while improving convenience in handling and storage.

[0018] The substrate in the gas reactive film composite of the present invention has a specific low moisture permeability. The moisture permeability of the substrate is 7 g / m ２ Less than 24 h, preferably 4 g / m ２ 24 hours or less, more preferably 1 g / m ２The lower limit of the moisture permeability is not particularly limited, and ideally it is 0 g / m ２ The moisture permeability of the substrate can be measured in accordance with JIS Z0208 (cup method).

[0019] In many cases, atmospheric moisture plays a major role in the deterioration of the light-emitting layer of a gas-reactive film composite. Specifically, the light-emitting layer is often deteriorated by phenomena such as the intrusion of moisture from the outside air when it is required to prevent moisture from entering the light-emitting layer, and the evaporation of moisture from the light-emitting layer to the outside when it is required to retain moisture within the light-emitting layer. Therefore, by using a substrate with such a specific low moisture permeability, it is possible to facilitate the storage and handling of the gas-reactive film composite and to suppress undesired intrusion of moisture from the outside air and undesired evaporation of moisture from the light-emitting layer to the outside.

[0020] In a preferred example, the substrate has either an average light transmittance at a wavelength of 300 to 400 nm or an average light transmittance at a wavelength of 400 to 750 nm that falls within a specific high range. More preferably, both of these fall within the specific high range. The average light transmittance of the substrate at a wavelength of 300 to 400 nm is preferably 80% or more, more preferably 85% or more, and even more preferably 87% or more. The upper limit of the average light transmittance at such wavelengths is ideally 100%, but in reality it can be set to a lower value, for example, 95% or less. The average light transmittance of the substrate at a wavelength of 400 to 750 nm is preferably 85% or more, more preferably 87% or more, and even more preferably 90% or more. The upper limit of the average light transmittance at such wavelengths is ideally 100%, but in reality it can be set to a lower value, for example, 95% or less. Since the excitation wavelength is often within the range of 300 to 400 nm, and the wavelength of the fluorescence or phosphorescence from the light-emitting layer is often within the range of 400 to 750 nm, a high light transmittance within this range allows for good analysis using a gas-reactive film multilayer. The light transmittance of the substrate can be obtained, for example, by measuring the total light transmittance at each wavelength within the measurement range using an ultraviolet-visible-near-infrared spectrophotometer (e.g., "V-770" manufactured by JASCO Corporation) with an integrating sphere and calculating the average.

[0021] The substrate may be a film-like member having a layered structure with a certain thickness. The thickness of the substrate is not particularly limited and can be appropriately adjusted to a range that has the mechanical strength to support the gas reaction film multilayer and maintains low moisture permeability and high light transmittance. The specific thickness is preferably 10 μm or more, more preferably 50 μm or more, and even more preferably 75 μm or more, and is preferably 300 μm or less, more preferably 200 μm or less, and even more preferably 100 μm or less.

[0022] The planar shape of the substrate in the gas-reactive film multilayer is not particularly limited and may be any desired shape. In a preferred example, the planar shape of the substrate is the same as or larger than the planar shape of the light-emitting layer, and is preferably such that one side of the light-emitting layer is entirely covered, from the viewpoint of achieving good protection of the light-emitting layer.

[0023] <Substrate Material: Alicyclic Structure-Containing Polymer> The substrate material is preferably a material that can achieve a specific low moisture permeability of the substrate at a desired substrate thickness. Specifically, a material that can achieve the desired low moisture permeability described above when molded into a substrate with a thickness that is thinner than a certain level is preferred. More specifically, the moisture permeability of the material constituting the substrate is preferably 7 g / m or less when molded into a film with a thickness of 100 μm. ２ Less than 24 h, preferably 4 g / m ２ 24 hours or less, more preferably 1 g / m ２ The lower limit of the moisture permeability is not particularly limited, and ideally it is 0 g / m ２ ・24 hours.

[0024] As the resin constituting the substrate having the above-mentioned specific low moisture permeability and high light transmittance, a resin having the above-mentioned properties can be appropriately selected from known resins and used. In particular, many resins included in the category of resins containing alicyclic structure-containing polymers have such low moisture permeability and high light transmittance and can be easily molded into a film having sufficient mechanical strength. Therefore, it is preferable to select an appropriate resin from among resins containing alicyclic structure-containing polymers.

[0025] In many cases, resin materials containing an alicyclic structure-containing polymer have low moisture permeability and high light transmittance, as well as low moisture absorption, low outgassing (a phenomenon in which components contained in a resin become gas and are released from the molded product after the resin is molded into the shape of a member such as a film), and low autofluorescence. Therefore, a resin containing an alicyclic structure-containing polymer is a material that can be particularly useful as a substrate in the present invention.

[0026] The alicyclic structure-containing polymer may have a cyclic structure in its molecule. Usually, the alicyclic structure-containing polymer has an alicyclic structure in the repeating unit of the polymer. The alicyclic structure-containing polymer may be a polymer having an alicyclic structure in the main chain, a polymer having an alicyclic structure in the side chain, a polymer having alicyclic structures in the main chain and the side chain, or a mixture of two or more of these in any ratio. From the viewpoint of mechanical strength, the alicyclic structure-containing polymer is preferably a polymer having an alicyclic structure in the main chain.

[0027] Examples of the alicyclic structure include saturated alicyclic hydrocarbon (cycloalkane) structures and unsaturated alicyclic hydrocarbon (cycloalkene, cycloalkyne) structures. Among these, from the viewpoint of mechanical strength, cycloalkane structures and cycloalkene structures are preferred, and cycloalkane structures are particularly preferred.

[0028] The number of carbon atoms constituting the alicyclic structure is preferably 4 or more, more preferably 5 or more, per one alicyclic structure, and is preferably 30 or less, more preferably 20 or less, particularly preferably 15 or less, and when this number is within this range, mechanical strength, heat resistance, and moldability are well balanced.

[0029] In the alicyclic structure-containing polymer, the proportion of repeating units having an alicyclic structure to all repeating units is preferably 55% by weight or more, more preferably 70% by weight or more, and even more preferably 90% by weight or more. A proportion of repeating units having an alicyclic structure to all repeating units in this range is preferred from the viewpoints of high light transmittance and heat resistance.

[0030] Examples of the alicyclic structure-containing polymer include known crystalline and amorphous alicyclic structure-containing polymers. More specific examples thereof include norbornene-based polymers; monocyclic alicyclic structure-containing polymers, cyclic conjugated diene-based polymers, vinyl alicyclic hydrocarbon-based polymers, and hydrogenated products thereof; and hydrogenated vinyl aromatic hydrocarbon polymers. Among these, one or more selected from the group consisting of norbornene-based polymers; vinyl alicyclic hydrocarbon-based polymers and hydrogenated products thereof; and hydrogenated vinyl aromatic hydrocarbon polymers are more preferred because of their good light transmittance.

[0031] Examples of norbornene-based polymers include ring-opening polymers of monomers having a norbornene structure and their hydrogenated products; addition polymers of monomers having a norbornene structure and their hydrogenated products.In addition, examples of ring-opening polymers of monomers having a norbornene structure include ring-opening homopolymers of one type of monomer having a norbornene structure, ring-opening copolymers of two or more types of monomers having a norbornene structure, and ring-opening copolymers of a monomer having a norbornene structure and any monomer copolymerizable therewith.In addition, examples of addition polymers of monomers having a norbornene structure include addition homopolymers of one type of monomer having a norbornene structure, addition copolymers of two or more types of monomers having a norbornene structure, and addition copolymers of a monomer having a norbornene structure and any monomer copolymerizable therewith. Among these, preferred are hydrogenated ring-opening polymers of monomers having a norbornene structure, addition copolymers of monomers having a norbornene structure and α-olefins, and hydrogenated addition copolymers of monomers having a norbornene structure and α-olefins; and more preferred are hydrogenated ring-opening copolymers of two or more monomers having a norbornene structure, addition copolymers of monomers having a norbornene structure and α-olefins, and hydrogenated addition copolymers of monomers having a norbornene structure and α-olefins.

[0032] Examples of monomers having a norbornene structure include bicyclo[2.2.1]hept-2-ene (common name: norbornene), tricyclo[4.3.0.1]hept-2-ene, and the like. ２，５ ]deca-3,7-diene (common name: dicyclopentadiene), 7,8-benzotricyclo[4.3.0.1 ２，５ ]dec-3-ene (common name: methanotetrahydrofluorene), tetracyclo[4.4.0.1 ２，５ .1 ７，１０]dodec-3-ene (common name: tetracyclododecene), and derivatives of these compounds (for example, those having a substituent on the ring). Examples of the substituent include an alkyl group, an alkylene group, and a polar group. These substituents may be the same or different, and a plurality of them may be bonded to the ring. The monomer having a norbornene structure may be used alone or in combination of two or more kinds in any ratio.

[0033] Examples of polar groups include heteroatoms and atomic groups having heteroatoms. Examples of heteroatoms include oxygen atoms, nitrogen atoms, sulfur atoms, silicon atoms, and halogen atoms. Specific examples of polar groups include carboxyl groups, carbonyloxycarbonyl groups, epoxy groups, hydroxyl groups, oxy groups, ester groups, silanol groups, silyl groups, amino groups, nitrile groups, and sulfonic acid groups.

[0034] Examples of monomers capable of ring-opening copolymerization with a monomer having a norbornene structure include monocyclic olefins such as cyclohexene, cycloheptene, and cyclooctene, and derivatives thereof; and cyclic conjugated dienes such as cyclohexadiene and cycloheptadiene, and derivatives thereof. The monomers capable of ring-opening copolymerization with a monomer having a norbornene structure may be used alone or in combination of two or more in any ratio.

[0035] A ring-opening polymer of a monomer having a norbornene structure can be produced, for example, by polymerizing or copolymerizing the monomer in the presence of a ring-opening polymerization catalyst.

[0036] In the addition copolymer of a monomer having a norbornene structure and an α-olefin, examples of the α-olefin include α-olefins having 2 to 20 carbon atoms, such as ethylene, propylene, and 1-butene, and derivatives thereof. Among these, ethylene is preferred. One type of α-olefin may be used alone, or two or more types may be used in combination in any ratio.

[0037] An addition polymer of a monomer having a norbornene structure can be produced, for example, by polymerizing or copolymerizing the monomer in the presence of an addition polymerization catalyst.

[0038] The hydrogenated products of the ring-opening polymer and the addition polymer described above can be produced, for example, by hydrogenating, preferably to 90% or more, the carbon-carbon unsaturated bonds in a solution of the ring-opening polymer and the addition polymer in the presence of a hydrogenation catalyst containing a transition metal such as nickel or palladium.

[0039] Examples of commercially available norbornene-based polymers include "ZEONOR" and "ZEONEX" manufactured by Zeon Corporation; "ARTON" manufactured by JSR Corporation; and "APEL" manufactured by Mitsui Chemicals, Inc.

[0040] Examples of vinyl alicyclic hydrocarbon polymers include polymers of vinyl alicyclic hydrocarbon monomers such as vinylcyclohexene and vinylcyclohexane, and their hydrogenated products; and hydrogenated products of the aromatic ring moieties of polymers of vinyl aromatic monomers. Furthermore, the polymer of a vinyl alicyclic hydrocarbon monomer may be a copolymer of a vinyl alicyclic hydrocarbon monomer and any monomer copolymerizable with the vinyl alicyclic hydrocarbon monomer. Furthermore, the polymer of a vinyl aromatic monomer may be a copolymer of a vinyl aromatic monomer and any monomer copolymerizable with the vinyl aromatic monomer. Examples of the copolymers include random copolymers and block copolymers. Examples of block copolymers include diblock copolymers, triblock copolymers, multiblock copolymers with higher order units, and gradient block copolymers.

[0041] The vinyl alicyclic hydrocarbon polymer is preferably a hydrogenated vinyl aromatic hydrocarbon polymer. The vinyl aromatic hydrocarbon polymer refers to a polymer containing a repeating unit [I] derived from an aromatic vinyl compound. The repeating unit derived from an aromatic vinyl compound refers to a repeating unit having a structure obtained by polymerizing an aromatic vinyl compound. However, in the present application, the polymer and its constituent units are not limited by their production method.

[0042] Examples of aromatic vinyl compounds corresponding to the repeating unit [I] include styrene; styrenes having an alkyl group having 1 to 6 carbon atoms as a substituent, such as α-methylstyrene, 2-methylstyrene, 3-methylstyrene, 4-methylstyrene, 2,4-dimethylstyrene, 2,4-diisopropylstyrene, 4-t-butylstyrene, and 5-t-butyl-2-methylstyrene; styrenes having a halogen atom as a substituent, such as 4-chlorostyrene, dichlorostyrene, and 4-monofluorostyrene; styrenes having an alkoxy group having 1 to 6 carbon atoms as a substituent, such as 4-methoxystyrene; styrenes having an aryl group as a substituent, such as 4-phenylstyrene; and vinyl naphthalenes such as 1-vinylnaphthalene and 2-vinylnaphthalene. These may be used alone, or two or more may be used in combination in any ratio. Among these, aromatic vinyl compounds not containing a polar group, such as styrene and styrenes having an alkyl group having 1 to 6 carbon atoms as a substituent, are preferred because they can reduce hygroscopicity, and styrene is particularly preferred because of its ease of industrial availability.

[0043] As a particularly preferred example of the alicyclic structure-containing polymer, the polymer containing the repeating unit [I] derived from an aromatic vinyl compound is preferably a specific block copolymer [D]. The block copolymer [D] is a block copolymer consisting of a polymer block [A] and a polymer block [B] or a polymer block [C]. The polymer block [A] is a polymer block mainly composed of the repeating unit [I] derived from an aromatic vinyl compound. The polymer block [B] is a polymer block mainly composed of the repeating unit [I] derived from an aromatic vinyl compound and the repeating unit [II] derived from a linear conjugated diene compound. The polymer block [C] is a polymer block mainly composed of the repeating unit [II] derived from a linear conjugated diene compound. Here, the "main component" refers to a component that accounts for 50% by weight or more of the polymer block. The proportion of the main component in the polymer block is preferably 80% by weight or more, more preferably 90% by weight or more, and even more preferably 100% by weight. The repeating unit derived from a linear conjugated diene compound refers to a repeating unit having a structure obtained by polymerizing a linear conjugated diene compound.

[0044] Examples of the chain conjugated diene compound corresponding to the repeating unit [II] include 1,3-butadiene, isoprene, 2,3-dimethyl-1,3-butadiene, and 1,3-pentadiene. These may be used alone or in combination of two or more in any ratio. The chain conjugated diene compound may be linear or branched.

[0045] The hydrogenated vinyl aromatic hydrocarbon polymer is a hydrogenated polymer containing a repeating unit [I] derived from an aromatic vinyl compound. The hydrogenated polymer containing a repeating unit [I] derived from an aromatic vinyl compound is preferably a specific hydrogenated block copolymer [E]. The hydrogenated block copolymer [E] is a hydrogenated product of the aforementioned block copolymer [D].

[0046] A hydrogenated vinyl aromatic hydrocarbon polymer is a substance obtained by hydrogenating the unsaturated bonds of a vinyl aromatic hydrocarbon polymer. Here, the unsaturated bonds of the vinyl aromatic hydrocarbon polymer to be hydrogenated include both carbon-carbon unsaturated bonds in the main chain and side chains of the polymer and carbon-carbon unsaturated bonds in the aromatic rings.

[0047] The hydrogenated product can be produced, for example, by hydrogenating the unsaturated bonds of the polymer, preferably to 90% or more, in a solution of the vinyl aromatic hydrocarbon polymer in the presence of a hydrogenation catalyst containing a transition metal such as nickel or palladium.

[0048] The above-mentioned alicyclic structure-containing polymers are mainly amorphous polymers. Other preferred examples of crystalline alicyclic structure-containing polymers include the following polymers (α) to (δ). These crystalline polymers can exhibit particularly low moisture permeability and high oil resistance (durability against oil on the surface of hands during handling) among alicyclic structure-containing polymers. Furthermore, among these, polymer (β) is particularly preferred. Polymer (α): A ring-opening polymer of a cyclic olefin monomer, which has crystallinity. Polymer (β): A hydrogenated product of polymer (α), which has crystallinity. Polymer (γ): An addition polymer of a cyclic olefin monomer, which has crystallinity. Polymer (δ): A hydrogenated product of polymer (γ), etc., which has crystallinity.

[0049] More specifically, the crystalline alicyclic structure-containing polymer is preferably a crystalline ring-opening polymer of dicyclopentadiene, or a crystalline hydrogenated ring-opening polymer of dicyclopentadiene, and particularly preferably a crystalline hydrogenated ring-opening polymer of dicyclopentadiene. Here, the ring-opening polymer of dicyclopentadiene refers to a polymer in which the proportion of dicyclopentadiene-derived structural units to all structural units is usually 50% by weight or more, preferably 70% by weight or more, more preferably 90% by weight or more, and even more preferably 100% by weight.

[0050] The crystalline alicyclic structure-containing polymer preferably has a syndiotactic structure, and more preferably has a high degree of syndiotactic stereoregularity. This can increase the crystallinity of the polymer, thereby particularly increasing durability. The degree of syndiotactic stereoregularity of the crystalline alicyclic structure-containing polymer can be expressed by the ratio of racemo-dyads in the crystalline alicyclic structure-containing polymer. The specific ratio of racemo-dyads is preferably 51% or more, more preferably 60% or more, and particularly preferably 70% or more. The ratio of racemo-dyads can be measured by the following method.

[0051] Orthodichlorobenzene-d ４The polymer was decoupling by the inverse-gated decoupling method at 200°C using １３ C-NMR measurement is carried out. １３ As a result of C-NMR measurement, orthodichlorobenzene-d ４ Using the peak at 127.5 ppm as the reference shift, the signal at 43.35 ppm from the meso dyad and the signal at 43.43 ppm from the racemo dyad are identified. Based on the intensity ratio of these signals, the proportion of racemo dyads in the polymer can be determined.

[0052] The crystalline alicyclic structure-containing polymer may be used alone or in combination of two or more kinds in any ratio.

[0053] A crystalline alicyclic structure-containing polymer can usually have a high degree of crystallinity due to crystallization. The specific range of the degree of crystallinity can be appropriately selected depending on the desired performance, but is preferably 10% or more, more preferably 15% or more, and particularly preferably 30% or more. By making the degree of crystallinity equal to or greater than the lower limit of the above range, properties such as low moisture permeability and high oil resistance can be obtained. The degree of crystallinity of the polymer can be measured by X-ray diffraction.

[0054] The crystalline alicyclic structure-containing polymer can be produced by any method, for example, the method described in WO 2016 / 067893.

[0055] The polymers described above that can be used as the alicyclic structure-containing polymer may contain a silicon atom-containing polar group in addition to the molecular structure described above.Preferred examples of polymers containing such a silicon atom-containing polar group include the hydrogenated vinyl aromatic hydrocarbon polymer described above, modified with a silicon atom-containing polar group.When a polymer containing a silicon atom-containing polar group is used as the alicyclic structure-containing polymer, the adhesion between the part containing the polymer containing the silicon atom-containing polar group and other members can be improved.

[0056] Hereinafter, the polymer used in the reaction to obtain the modified product may be referred to as a "pre-reaction polymer." The modified product may have a structure obtained by, for example, graft polymerization of the pre-reaction polymer with a compound having a silicon atom-containing polar group as a monomer. However, the modified product is not limited by its production method. The silicon atom-containing polar group is preferably an alkoxysilyl group.

[0057] Examples of compounds having a silicon atom-containing polar group that can be used as a monomer for graft polymerization include compounds having an alkoxysilyl group, and specific examples thereof include ethylenically unsaturated silane compounds having an alkoxysilyl group, such as vinyltrimethoxysilane, vinyltriethoxysilane, allyltrimethoxysilane, allyltriethoxysilane, dimethoxymethylvinylsilane, diethoxymethylvinylsilane, p-styryltrimethoxysilane, p-styryltriethoxysilane, 3-methacryloxypropyltrimethoxysilane, 3-methacryloxypropylmethyldimethoxysilane, 3-methacryloxypropyltriethoxysilane, 3-methacryloxypropylmethyldiethoxysilane, 3-acryloxypropyltrimethoxysilane, 3-acryloxypropyltriethoxysilane, and 2-norbornen-5-yltrimethoxysilane.

[0058] By reacting a pre-reaction polymer with a compound having a silicon atom-containing polar group, a silicon atom-containing polar group can be introduced into the pre-reaction polymer, thereby obtaining a modified product having a silicon atom-containing polar group. When an alkoxysilyl group is introduced as the silicon atom-containing polar group, the amount of alkoxysilyl group introduced is preferably 0.1 parts by weight or more, more preferably 0.2 parts by weight or more, and even more preferably 0.3 parts by weight or more, relative to 100 parts by weight of the pre-reaction polymer, and is preferably 10 parts by weight or less, more preferably 5 parts by weight or less, and even more preferably 3 parts by weight or less. When the amount of alkoxysilyl group introduced falls within the above range, the degree of crosslinking between alkoxysilyl groups decomposed by water can be prevented from becoming excessively high, so the effect of the alkoxysilyl group can be maintained at a high level. Examples of substances having alkoxysilyl groups used to introduce alkoxysilyl groups and modification methods include those described in WO 2015 / 099079.

[0059] The amount of polar groups introduced is １ When measuring the amount of polar groups introduced, if the amount introduced is small, the number of integration times can be increased.

[0060] Introducing an alkoxysilyl group as a polar group into a pre-reaction polymer is called silane modification. In the silane modification, the alkoxysilyl group may be bonded directly to the pre-reaction polymer, or may be bonded via a divalent organic group such as an alkylene group. Hereinafter, the polymer obtained by silane modification of the pre-reaction polymer is also referred to as a "silane-modified polymer."

[0061] The silane-modified polymer is preferably one or more polymers selected from a silane-modified hydrogenated styrene-butadiene block copolymer, a silane-modified hydrogenated styrene-butadiene-styrene block copolymer, a silane-modified hydrogenated styrene-isoprene block copolymer, and a silane-modified hydrogenated styrene-isoprene-styrene block copolymer.

[0062] The resin constituting the substrate may contain one type of polymer or two or more types of polymers.

[0063] The weight-average molecular weight Mw of the polymer contained in the resin constituting the substrate is preferably 10,000 or more, more preferably 15,000 or more, particularly preferably 20,000 or more, and is preferably 100,000 or less, more preferably 80,000 or less, particularly preferably 50,000 or less. When the weight-average molecular weight is in this range, the mechanical strength and moldability of the resin are well balanced.

[0064] The molecular weight distribution (Mw / Mn) of the polymer contained in the resin constituting the substrate is preferably 1.2 or more, more preferably 1.5 or more, particularly preferably 1.8 or more, and preferably 3.5 or less, more preferably 3.0 or less, particularly preferably 2.7 or less. Here, Mn represents the number average molecular weight. When the molecular weight distribution is equal to or greater than the lower limit of the above range, the productivity of the polymer can be increased and the production cost can be reduced. On the other hand, when it is equal to or less than the upper limit, the amount of low molecular weight components is reduced, and the stability of the substrate containing the polymer can be improved.

[0065] The weight average molecular weight (Mw) and number average molecular weight (Mn) can be measured using gel permeation chromatography (GPC). Solvents used in GPC include cyclohexane, toluene, and tetrahydrofuran. When using GPC, the weight average molecular weight is measured as a relative molecular weight, for example, in terms of polyisoprene or polystyrene.

[0066] The weight ratio (content) of the polymer in the resin constituting the substrate is preferably 50% by weight or more, more preferably 60% by weight or more, even more preferably 70% by weight or more, still more preferably 80% by weight or more, and particularly preferably 90% by weight or more. The upper limit is usually 100% by weight or less, and may be 99% by weight or less.

[0067] The resin constituting the substrate may contain other optional components in combination with the polymer such as the alicyclic structure-containing polymer, as long as the effects of the present invention are not significantly impaired. Examples of the optional components include additives such as colorants such as pigments and dyes; fluorescent brighteners; dispersants; heat stabilizers; light stabilizers; ultraviolet absorbers; antistatic agents; antioxidants; and lubricants. One type of optional component may be used alone, or two or more types may be used in combination in any ratio.

[0068] <Gas-Reactive Film Multilayer: Luminescent Layer> The luminescent layer is a layer containing a gas-reactive luminescent material. The gas-reactive luminescent material is a material that, upon reacting with a gas to be detected, acquires the property of changing the degree of luminescence depending on the amount of reaction. Using a luminescent layer containing such a material, it is possible to qualitatively analyze whether or not the gas to be detected has come into contact with the luminescent layer, or to quantitatively analyze the amount of the gas to be detected that has come into contact with the luminescent layer. In this case, the change in the degree of luminescence may be either an increase in the degree of luminescence upon reaction with the gas, or a decrease in the degree of luminescence upon reaction with the gas.

[0069] In a preferred example, the gas-responsive luminescent material is a material that reacts with skin gases to be detected. Skin gases are gases that can be emitted from the skin of human and non-human living organisms. Skin gases can follow various emission routes, such as those that are emitted from blood in subcutaneous capillaries through the blood vessel walls and skin, those that are emitted from sebaceous glands on the skin, and those that are emitted from gas-generating sources such as resident bacteria present on the skin. The presence or absence and amount of skin gas emission can vary depending on the health state of the living organism, and are therefore useful as information about the living organism.

[0070] Specific examples of skin gases include acetone (which can be an indicator of diabetes and fat metabolism), ammonia (which can be an indicator of various liver diseases and protein metabolism), isoprene (which can be an indicator of sleep), methyl mercaptan (which can be an indicator of liver disease), carbon monoxide (which can be an indicator of oxidative stress), ethanol (which can be an indicator of alcohol consumption), trimethylamine (which can be an indicator of kidney diseases such as renal failure), and nitric oxide (which can be an indicator of asthma and gas poisoning). The gas-reactive luminescent material reacts with these gases, making it possible to obtain biological information corresponding to the gas.

[0071] In a preferred example, the gas responsive luminescent material is a material whose photoluminescent properties change upon reaction with a gas to be detected. That is, the gas responsive luminescent material in such a preferred example is a material whose photoluminescent properties increase or decrease upon contact with a gas to be detected. Such a change may change the molecular structure of the gas responsive luminescent material, and the material may become a different substance. However, for convenience in this application, and as long as it is clear from the context, the material before and after such a change will be referred to as the gas responsive luminescent material without distinction.

[0072] The photoluminescent property of the material is the property of emitting light in response to irradiation with excitation light. Such light emission can be fluorescence or phosphorescence. By measuring the amount of light emission, it is possible to qualitatively analyze whether or not the target gas has come into contact with the light-emitting layer, or to quantitatively analyze the amount of target gas that has come into contact with the light-emitting layer.

[0073] The light-emitting layer may contain any material in addition to the gas-responsive light-emitting material, specifically, a filler material for holding the gas-responsive light-emitting material in the layer.

[0074] The gas-responsive luminescent material and other optional materials constituting the luminescent layer may be any known material. Specifically, any known material that can be used to detect specific components in the exhaled breath or skin gas of a living body may be used. Examples of gas-responsive luminescent materials and excipient materials include those described in Patent Documents 1 to 4.

[0075] More specifically, an example of a gas-reactive luminescent material is a combination of an enzyme and a coenzyme whose luminescence properties can be changed by an enzymatic reaction, as described in Patent Document 2. Even more specifically, when ethanol is to be detected, a combination of ADH (primary alcohol dehydrogenase) and NAD ＋ a combination of ADH and NADH (oxidized nicotinamide adenine dinucleotide) when acetaldehyde is to be detected; a combination of S-ADH (secondary alcohol dehydrogenase) and NADH when acetone is to be detected; and a combination of S-ADH and NADH when 2-propanol is to be detected. ＋ A combination of ALDH (aldehyde dehydrogenase) and NAD when acetaldehyde or 2-nonenal is to be detected. ＋ and when formaldehyde is to be detected, FALDH (formaldehyde dehydrogenase) and NAD ＋ A combination of the following is included.

[0076] In these combinations of enzyme and coenzyme, NADH is converted to NAD by contact of the enzyme with gas. ＋ This change occurs when NADH is converted to NAD. ＋ The difference in photoluminescent properties of NADH and NADH (i.e., NADH emits fluorescence at wavelengths of 450 to 510 nm, more specifically, around 491 nm, when excited by light of wavelength 340 nm, whereas NADH ＋ The analysis can be performed by detecting the fluorescent protein using fluorescent dyes (which do not emit fluorescence).

[0077] The proportion of the gas-reactive luminescent material in the luminescent layer can be adjusted to a suitable proportion depending on the type and application of the luminescent material used. The proportion of the gas-reactive luminescent material in 100% by weight of the luminescent layer is preferably 0.01% by weight or more, more preferably 0.1% by weight or more, and is preferably 60% by weight or less, more preferably 50% by weight or less.

[0078] Examples of the filler material constituting the luminescent layer include various materials capable of incorporating the gas-responsive luminescent material and forming a layered outer shape. More specific examples include polymers, metals, metal compounds, and composites thereof. Polymers include natural polymers, semi-synthetic polymers, and synthetic polymers. Examples of natural polymers include cellulose and dextran. Examples of semi-synthetic polymers include regenerated cellulose, chemically modified cellulose, and cellulose derivatives such as methyl cellulose, carboxymethyl cellulose, and cellulose acetate. Examples of synthetic polymers include polyolefins such as polyethylene and polypropylene, polyesters such as polyethylene terephthalate and polyethylene naphthalate, acrylic polymers such as polyacrylonitrile and polyacrylamide, polyvinyl alcohol and its derivatives, polyethers such as polyethylene oxide and polyethylene glycol, polyurethanes, polyvinylpyrrolidone, and fluororesins such as polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), and ethylene-tetrafluoroethylene copolymer (ETFE). Examples of metals include titanium, aluminum, and stainless steel. Examples of metal compounds include metal oxides such as alumina.

[0079] The light-emitting layer is usually provided on one side of the substrate directly or via an optional layer. The thickness of the light-emitting layer is not particularly limited and can be appropriately adjusted to a thickness suitable for observing the reaction with the gas and the light emission. Specifically, the thickness is preferably 1 μm or more, and preferably 300 μm or less.

[0080] <Gas-Reactive Film Multilayer: Optional Components> The gas-reactive film multilayer of the present invention may include optional components in addition to the substrate and the light-emitting layer. Examples of the optional components include an adsorbent layer, an adhesive layer, a protective layer, a separator, a substrate with ventilation holes, a frame, and a support substrate.

[0081] <Adsorbent Layer> The adsorbent layer is a layer that adsorbs fluids other than the gas to be detected (i.e., gases, liquids, or both). By providing the gas-reactive film composite with the adsorbent layer, it is possible to prevent fluids that adversely affect the analysis from being absorbed by the light-emitting layer.

[0082] As an example, if moisture other than the gas being detected is emitted from the living body being analyzed and the moisture interferes with the measurement of the gas being detected, the gas-reactive film composite can be provided with a moisture-absorbing layer as an adsorbent layer, which will absorb the moisture emitted from the skin, thereby reducing the amount of moisture that has a negative effect on the light-emitting layer.

[0083] As another example, if the gas to be detected is a basic gas such as ammonia, and in addition to the basic gas, an acidic gas such as acetic acid may be emitted from the living body being analyzed, the gas-reactive film composite can be provided with an adsorbent layer that absorbs acidic gases, so that the adsorbent layer absorbs the acidic gas emitted from the subject to be analyzed, thereby reducing the amount of acidic gas that has a negative effect on the light-emitting layer.

[0084] Examples of materials that make up the adsorbent layer include a sheet in which silica gel or the like is sandwiched between nonwoven fabric of resin fibers such as polypropylene, or a sheet impregnated with a substance that can function as an adsorbent (for example, basic substances such as potassium hydroxide and sodium hydroxide as adsorbents for acidic gases).

[0085] The adsorbent layer is preferably provided on the same side of the substrate as the light-emitting layer, so that the light-emitting layer and the adsorbent layer coexist in the region between the surface of the object to be analyzed and the substrate, thereby enabling the above-mentioned effect of adsorption of the object gas to be detected to be effectively exhibited.

[0086] The thickness of the adsorbent layer is not particularly limited and can be appropriately adjusted to a thickness suitable for observing the reaction with the gas and the luminescence. Specifically, the thickness is preferably 1 μm or more, and on the other hand, preferably 300 μm or less.

[0087] <Adhesive layer> The adhesive layer is a layer that, due to its adhesiveness, makes it easy to place the gas reactive film multilayer on the surface of the object to be analyzed. The material constituting the adhesive layer is not particularly limited, and a material having the desired adhesiveness can be appropriately selected. For example, a material known as a medical adhesive can be appropriately selected and used as the material for the adhesive layer.

[0088] The adhesive layer is preferably provided on the same side of the substrate as the light-emitting layer. Additionally, the adhesive layer is preferably provided on the periphery of the gas-reactive film composite in terms of its planar positional relationship with the gas-reactive film composite. By arranging the adhesive layer in this manner, the adhesive layer further surrounds the outer periphery of the region where the light-emitting layer and the adsorbent layer coexist in the region between the surface of the analysis target and the substrate, thereby forming a sealed region that includes the light-emitting layer and the adsorbent layer. This allows the effects of the light-emitting layer and the adsorbent layer to be more effectively achieved.

[0089] <Protective Layer> The protective layer is a layer provided to suppress deterioration of the gas-reactive film composite, particularly deterioration of the surface of the substrate. For example, if the gas-reactive film composite is provided on the surface of the object to be analyzed for a long period of time, physical impacts may be applied to the substrate-side surface of the composite, causing deterioration such as scratches on the substrate, and changes in the optical properties of the substrate may occur. Such changes in optical properties may interfere with the detection of fluorescence or phosphorescence from the light-emitting layer. Here, by providing the gas-reactive film composite with a protective layer, such deterioration can be suppressed, making it easier to perform accurate analysis.

[0090] The protective layer may be provided for the purpose of suppressing the intrusion of fluids other than moisture from the outside air that need to be prevented from flowing into the light-emitting layer. For example, if the light-emitting layer is susceptible to deterioration due to the inflow of oxygen in addition to moisture, and the base material has a low ability to suppress oxygen permeation, a layer with a high ability to suppress oxygen permeation may be provided as the protective layer. By providing such a protective layer, it is possible to suppress the permeation of both moisture and oxygen.

[0091] The material constituting the protective layer is not particularly limited, and a material capable of exhibiting the desired protective performance can be appropriately selected. For example, a film known as a hard coat film for optical components can be appropriately selected and used as the protective layer. Specific materials constituting the protective layer include polyvinyl alcohol, which has high oxygen barrier properties, and inorganic materials with high barrier properties against various gases. Preferred examples of inorganic materials include metals (including semimetals); metal compounds such as metal oxides, metal nitrides, and metal oxynitrides; and DLC (diamond-like carbon). Examples of the metal include aluminum and silicon.

[0092] The protective layer is preferably provided on the side of the substrate opposite to the side on which the light-emitting layer is provided. For example, if the protective layer itself has sufficient scratch resistance and light transmittance, its presence may not interfere with the detection of fluorescence or phosphorescence from the light-emitting layer. In this case, the gas-reactive film multilayer can be subjected to the detection process with the protective layer still provided. As another example, if the protective layer can protect the substrate but is easily scratched, or if the protective layer does not have sufficient light transmittance, the protective layer may be peeled off before detecting fluorescence or phosphorescence from the light-emitting layer.

[0093] <Separator> The separator is a layer provided in contact with the adhesive surface of the gas reactive film multilayer. The separator can protect the adhesive surface during the period prior to providing the gas reactive film multilayer on the surface of the analysis target. Such protection can suppress adhesion of the gas reactive film multilayer to objects other than the target during that period.

[0094] In addition, when the separator has a moisture permeability at least as low as that of the substrate, it is possible to suppress undesired changes in the moisture content in the light-emitting layer during the period (intrusion of moisture from the outside air when it is required to prevent moisture from entering the light-emitting layer, and evaporation of moisture from the light-emitting layer to the outside when it is required to retain moisture in the light-emitting layer). As a result, it is possible to suppress adverse effects on analysis due to changes in moisture content during the period, and it becomes possible to store the gas-reactive film multilayer for a long period during the period without requiring stringent packaging.

[0095] Usually, the separator is peeled off from the gas reactive film composite before the gas reactive film composite is placed on the surface of the object to be analyzed, and the gas reactive film composite can be easily placed by attaching the adhesive surface exposed by the peeling to the surface of the object to be analyzed.

[0096] The material constituting the separator is not particularly limited, and a material capable of exhibiting the desired release performance and other performances can be appropriately selected. For example, a film known as a separator for optical components having adhesive properties or a film made of the same material as the substrate can be appropriately selected to exhibit the desired performances and used as the separator.

[0097] <Substrate with Ventilated Holes> In some examples, the gas-reactive film multi-layer may include a substrate with vent holes between the substrate and the light-emitting layer. The substrate with vent holes is a substrate having holes penetrating from its front surface to its back surface. In the present invention, the substrate with vent holes is a separate component from the substrate.

[0098] At some point during the period when the gas-reactive film composite is placed on the surface of the subject to be analyzed, it may be necessary to vent the fluid within the sealed region. For example, in order to effectively capture a large amount of gas emitted from the skin with the light-emitting layer, or to prevent the gas-reactive film composite from falling off due to expansion of the sealed region, it may be necessary to vent the gas within the region (the gas that was present in the region when the film composite was placed on the subject to be analyzed, and the remaining gas that has reacted with the light-emitting layer from the skin) from the surface of the light-emitting layer opposite the skin. In such cases, the substrate can be peeled off from the substrate with ventilation holes to expose the ventilation holes, thereby connecting the sealed region to the outside and achieving fluid venting. If the substrate and the substrate with ventilation holes are attached in a manner that allows re-attachment after peeling, the substrate can be re-attached to the substrate with ventilation holes as needed, and the region can be re-sealed.

[0099] The material constituting the substrate with ventilation holes is not particularly limited, and a material capable of exhibiting the desired performance can be appropriately selected. From the viewpoint of facilitating detection of fluorescence or phosphorescence from the light-emitting layer when the substrate with ventilation holes is provided, it is preferable that the substrate with ventilation holes has a light transmittance equal to or higher than that of the substrate. From this viewpoint, it is preferable that the material constituting the substrate with ventilation holes is the same material as the substrate. However, since the substrate with ventilation holes is a component that is intended to allow ventilation from its front surface to its back surface, it is not required to have a moisture permeability as low as that of the substrate.

[0100] <Other Optional Components> The gas-reactive film composite of the present invention may include, as optional components other than those described above, components such as a frame, a support substrate, etc., for forming the gas-reactive film composite into a desired structure. Materials for forming these components may be appropriately selected from materials that have the desired mechanical strength and little effect on the reaction between the gas and the light-emitting layer.

[0101] <Shape of Gas-Reactive Film Composite> The structure of the gas-reactive film composite of the present invention may be any structure as long as the substrate and the light-emitting layer are in a layered shape. The planar shape of the gas-reactive film composite (i.e., the shape when observed from its thickness direction) may be any shape, such as a circle, a rectangle, or a shape that conforms to the shape of the object to be measured. The gas-reactive film composite may also have a flat shape that conforms to a flat surface, or a curved shape. For example, the gas-reactive film composite may have a curved shape that conforms to the shape of a non-flat object to be measured.

[0102] <Specific examples of the structure of the gas-reactive film multilayer, and the method for analyzing skin gases> The gas-reactive film multilayer of the present invention can be preferably used in the method for analyzing skin gases described below. Hereinafter, the method for analyzing skin gases will be described as the method for analyzing skin gases of the present invention, and specific examples of the structure of the gas-reactive film multilayer of the present invention will also be described.

[0103] The skin gas analysis method of the present invention comprises the following steps 1 to 4. The skin gas analysis method of the present invention may further comprise the following step 3. Step 1: A step of preparing the gas-reactive film composite of the present invention described above. Step 2: A step of placing the gas-reactive film composite on the skin of a subject to cause the skin gas to react with the gas-reactive luminescent material in the gas-reactive film. Step 3: A step after step 2 and before step 4, of sealing the gas-reactive luminescent material with which the skin gas has reacted, with a sealing substrate. Step 4: A step of irradiating the gas-reactive luminescent material with excitation light and detecting fluorescence or phosphorescence emitted from the gas-reactive luminescent material.

[0104] Fig. 1 is a longitudinal cross-sectional view schematically illustrating an example of a gas-reactive film composite of the present invention. In Fig. 1, gas-reactive film composite 100 includes substrate 111 and light-emitting layer 121 provided in contact with one surface 111D of substrate 111. In this example, light-emitting layer 121 is shaped to contact the entire surface 111D.

[0105] The substrate 111 is made of resin and has a moisture permeability of 7 g / m ２On the other hand, in this example, the light-emitting layer 121 includes a light-emitting material, and the light-emitting material is a material whose photoluminescent properties change when it reacts with skin gas emitted from the skin of the living body being measured.

[0106] In this example, gas-reactive film composite 100 is used to implement the skin gas analysis method of the present invention. In step 2, gas-reactive film composite 100 is placed so that surface 121D on the light-emitting layer 121 side is in contact with the skin of a living body to be analyzed. When gas is emitted from the skin, the gas comes into contact with or is absorbed by light-emitting layer 121, and the light-emitting material in light-emitting layer 121 reacts with the gas. As a result, the photoluminescent properties of the light-emitting material change depending on the amount of gas.

[0107] Gas-reactive film composite 100, having substrate 111 of a specific material that satisfies the above-described requirements, can suppress changes in the moisture content of light-emitting layer 221 during step 2 (such as moisture penetration into light-emitting layer 221 from surface 111U on substrate 111 side when moisture penetration into light-emitting layer 221 is required, or moisture evaporation from light-emitting layer 221 through substrate 111 to the outside when moisture is required to be retained in light-emitting layer 221). As a result, adverse effects of moisture on analysis can be suppressed. This feature is particularly useful, for example, when the duration of step 2 is long and there are frequent exposures to moisture despite the requirement to prevent moisture penetration into light-emitting layer 221 during that time, or when the duration of step 2 is long and there is a dry external environment despite the requirement to prevent moisture evaporation from light-emitting layer 221 during that time. More specifically, this feature is useful when the subject to be measured is a human, the duration of step 2 is a long period of time, such as one day or more, and although it is required to prevent moisture from entering the light-emitting layer 221, there are many opportunities for water to come into contact with surface 111U of the gas-reactive film composite 100 due to daily activities such as bathing.

[0108] Fig. 2 is a longitudinal cross-sectional view schematically illustrating another example of the gas reactive film composite of the present invention. In Fig. 2, gas reactive film composite 200 includes substrate 111 and light-emitting layer 221 provided in contact with one surface 111D of substrate 111. Substrate 111 is the same as that included in gas reactive film composite 100 in Fig. 1. Light-emitting layer 221 is made of the same material as light-emitting layer 121 included in gas reactive film composite 100 in Fig. 1. However, light-emitting layer 221 differs in shape from light-emitting layer 121, having a shape that contacts only a partial area inside surface 111D.

[0109] Gas reactive film composite 200 further includes separator 251 provided in contact with surface 221D of light-emitting layer 221 opposite substrate 111; and protective layer 212 provided in contact with surface 111U of substrate 111 opposite light-emitting layer 221. Gas reactive film composite 200 also includes adsorbent layer 241 and adhesive layer 231 between substrate 111 and separator 251. In this example, adsorbent layer 241 is provided adjacent to the outer side of light-emitting layer 221, and adhesive layer 231 is provided adjacent to the outer side of adsorbent layer 241. That is, in terms of planar positional relationship, adhesive layer 231 is provided on the periphery of gas reactive film composite 200, adsorbent layer 241 is provided inside thereof, and light-emitting layer 221 is provided further inside thereof.

[0110] When using gas-reactive film composite 200, prior to subjecting it to step 2, separator 251 is peeled off to expose surface 221D on which luminescent layer 221, adhesive layer 231, and adsorbent layer 241 are present. Then, in step 2, gas-reactive film composite 200 is placed so that surface 221D contacts the skin of the living body to be analyzed. When gas is released from the skin, the gas comes into contact with or is absorbed by luminescent layer 221, and the luminescent material in luminescent layer 221 reacts with the gas. As a result, the photoluminescent properties of the luminescent material change depending on the amount of gas.

[0111] Gas reactive film composite 200 is easier to handle due to the inclusion of separator 251. Specifically, by providing separator 251, adhesion of composite 200 to objects other than the installation target can be suppressed during the period before being subjected to step 2.

[0112] In addition, when the separator 251 has low moisture permeability at least as low as that of the substrate 111, it is possible to suppress changes in the moisture content in the light-emitting layer 221 during the period before subjecting it to step 2. As a result, it is possible to suppress adverse effects on analysis due to changes in the moisture content during that period, and it becomes possible to store the gas reactive film multilayer for a long period of time after the completion of step 1 until the implementation of step 2 without requiring strict packaging.

[0113] Gas-reactive film composite 200 can be easily placed on the surface of an object to be analyzed by providing adhesive layer 231. Specifically, with respect to gas-reactive film composite 100 shown in FIG. 1 , if light-emitting layer 121 is sufficiently adhesive to adhere to the skin, composite 100 can be placed on the surface of the skin simply by pressing composite 100 against the skin. However, if light-emitting layer 121 is not sufficiently adhesive to adhere to the skin, a step of attaching composite 100 to the skin using another member such as tape is required. In contrast, gas-reactive film composite 200 including adhesive layer 231 can be placed on the surface of the skin simply by pressing composite 200 against the skin, regardless of whether light-emitting layer 221 is sufficiently adhesive. This makes composite 200 easier to use and allows for greater freedom in selecting the composition of light-emitting layer 221.

[0114] By providing gas reactive film composite 200 with adsorbent layer 241, it is possible to prevent fluids that adversely affect analysis from being absorbed by light emitting layer 221. For example, if moisture other than the gas to be detected is dispersed from the skin and the moisture interferes with the measurement of the gas to be detected, by providing gas reactive film composite 200 with adsorbent layer 241, adsorbent layer 241 can absorb the moisture dispersed from the skin, and as a result, the amount of moisture that adversely affects light emitting layer 221 in step 2 can be reduced.

[0115] The analytical performance can be improved by positioning the adhesive layer 231 outside the light-emitting layer 221 and the adsorbent layer 241. That is, when the gas-reactive film composite 200 having such a positional relationship is placed in contact with the skin of the living body to be analyzed in step 2, the base material 111, the adhesive layer 231, and the skin form a sealed area, within which the light-emitting layer 221 and the adsorbent layer 241 are located. With such a positional relationship, the light-emitting layer 221 can effectively capture the gas emitted from the skin, thereby improving the analytical performance.

[0116] By providing protective layer 212, gas-reactive film composite 200 can suppress deterioration of the surface of substrate 111, thereby facilitating accurate analysis. For example, if step 2 is performed over a long period of time, physical impact may be applied to the substrate-side surface of composite 200, causing deterioration such as scratches on substrate 111 and resulting in changes in the optical properties of the substrate. Such changes in optical properties may interfere with the detection of fluorescence or phosphorescence from the light-emitting layer in step 4. Here, by providing gas-reactive film composite 200 with protective layer 212, such deterioration can be suppressed, making it easier to perform accurate analysis.

[0117] 3 is a longitudinal cross-sectional view schematically illustrating yet another example of a gas reactive film composite of the present invention. In FIG. 3, gas reactive film composite 300 includes substrate 111 and luminescent layer 221, and substrate 313 with ventilation holes disposed between substrate 111 and luminescent layer 221.

[0118] Gas reactive film composite 300 further includes separator 251 provided in contact with surface 221D of light-emitting layer 221 opposite substrate 111. Gas reactive film composite 300 also includes adsorbent layer 241 and adhesive layer 231 between substrate 111 and separator 251. In this example, adsorbent layer 241 is provided adjacent to the outer side of light-emitting layer 221, and adhesive layer 231 is provided adjacent to the outer side of adsorbent layer 241.

[0119] The substrate 111, the light-emitting layer 221, the adhesive layer 231, the adsorbent layer 241, and the separator 251 are the same as those provided in the gas reactive film composite 200 in Fig. 2. However, the substrate 111 is not in direct contact with the light-emitting layer 221, but is provided via a substrate 313 with ventilation holes.

[0120] The substrate 313 with ventilation holes has ventilation holes 314. The ventilation holes 314 are holes that penetrate from the front surface to the back surface of the substrate 313 with ventilation holes. In this example, the ventilation holes 314 are provided so that their openings are positioned across the light-emitting layer 221 and the adsorbent layer 241.

[0121] At some point during step 2, it may be necessary to vent the fluid within the sealed region of the gas-reactive film composite. For example, to effectively capture a large amount of gas emitted from the skin with light-emitting layer 221, or to prevent the gas-reactive film composite from falling off due to expansion of the region, it may be necessary to vent the gas within the region (gas that was present in the region when light-emitting layer 221 was initially placed on the subject of analysis, and the remaining gas that has been emitted from the skin and reacted with light-emitting layer 221) from the surface opposite the skin of light-emitting layer 221. In such cases, by peeling a part or all of substrate 111 from vented substrate 313 and exposing vent holes 314, the sealed region can be connected to the outside, thereby achieving fluid venting. If substrate 111 and vented substrate 313 are attached in a manner that allows them to be reattached after peeling, substrate 111 can be reattached to vented substrate 313 as needed, and the region can be resealed.

[0122] Fig. 4 is a longitudinal cross-sectional view schematically illustrating another example of a gas reactive film composite of the present invention. In Fig. 4, gas reactive film composite 400 includes substrate 111 and light-emitting layer 421 provided in contact with one surface 111D of substrate 111. In this example, light-emitting layer 421 has a shape that contacts only a partial area inside surface 111D.

[0123] Gas reactive film composite 400 further comprises a frame 461 provided in contact with the area of ​​surface 111D of substrate 111 outside light-emitting layer 421; an adsorbent layer 441 provided in the area inside the frame; an adhesive layer 431 provided in contact with the surface of frame 461 opposite substrate 111; a separator 251 provided in contact with the surface of adhesive layer 431 opposite substrate 111; and a protective layer 212 provided in contact with surface 111U of substrate 111 opposite light-emitting layer 421.

[0124] The substrate 111 is the same as that provided in the gas reactive film composite 100 in Fig. 1. The separator 251 is the same as that provided in the gas reactive film composite 200 in Fig. 2. The materials of the light-emitting layer 421, the adhesive layer 431, and the adsorbent layer 441 are the same as those of the light-emitting layer 221, the adhesive layer 231, and the adsorbent layer 241 provided in the gas reactive film composite 200 in Fig. 2. However, the shapes of the light-emitting layer 421, the adhesive layer 431, and the adsorbent layer 441 are different from those of the light-emitting layer 221, the adhesive layer 231, and the adsorbent layer 241.

[0125] Since the frame 461, the adhesive layer 431, and the adsorbent layer 441 are provided only in the area near the periphery of the gas reactive film composite 400, the gas reactive film composite 400 has a void 471 therein.

[0126] When using gas-reactive film composite 400, prior to subjecting it to step 2, separator 251 is peeled off to expose surface 431D of adhesive layer 431 facing separator 251. Then, in step 2, gas-reactive film composite 400 is placed so that surface 431D contacts the skin of the living body being analyzed. When gas is released from the skin, the gas enters voids 471 and then comes into contact with or is absorbed by luminescent layer 421, causing the luminescent material in luminescent layer 421 to react with the gas. As a result, the photoluminescent properties of the luminescent material change depending on the amount of gas.

[0127] Gas-reactive film composite 400 may have a structure with voids 471, which may allow analysis to be performed more advantageously in some cases. For example, direct contact of light-emitting layer 421 with the subject of analysis may be required because direct contact of light-emitting layer 421 with the skin surface of the subject of analysis may result in adverse phenomena such as deterioration, or because water vapor emitted from the skin may condense on the skin surface, which may then come into contact with light-emitting layer 421, resulting in adverse phenomena such as deterioration of light-emitting layer 421. In such cases, having a structure with voids 471 can reduce the occurrence of these adverse phenomena. Furthermore, having a structure with voids 471 can increase the rate at which fluids that adversely affect analysis are absorbed by adsorbent layer 441 before reaching light-emitting layer 421.

[0128] 5 is a longitudinal cross-sectional view schematically illustrating another example of a gas reactive film laminate of the present invention. In FIG. 5, gas reactive film laminate 500 includes frame 461 and support substrate 481 disposed between adhesive layer 431.

[0129] Gas reactive film composite 500 further comprises substrate 111, protective layer 212, light emitting layer 421, adhesive layer 431, adsorbent layer 441, separator 251, and frame 461. These are the same as those comprised in gas reactive film composite 400 in Fig. 4. However, adhesive layer 431 and frame 461 are not in direct contact with each other, but are provided via support substrate 481.

[0130] Support substrate 481 has hole 482. Hole 482 is a hole that penetrates support substrate 481 from the front surface to the back surface. By providing support substrate 481, the void inside gas reactive film composite 500 is divided into void 472U on the substrate 111 side and void 472D on the separator 251 side. Voids 472U and 472D become a pair of voids that are fluid-flow connected by hole 482.

[0131] Gas-reactive film composite 500, having such support substrate 481, can advantageously perform analysis in some cases. For example, direct contact of light-emitting layer 421 with the subject of analysis may be required because direct contact of light-emitting layer 421 with the skin surface of the subject of analysis may result in adverse phenomena such as deterioration, or because water vapor emitted from the skin may condense on the skin surface, causing adverse phenomena such as deterioration of light-emitting layer 421 when the condensed water comes into contact with light-emitting layer 421. In such cases, deformation of the gas-reactive film composite, such as bending, may reduce the distance between the skin surface and the light-emitting layer, potentially resulting in contact between them. Here, gas-reactive film composite 500 having support substrate 481 can avoid contact between the skin surface and light-emitting layer 421.

[0132] <Analysis Method: Step 1> Step 1 of the skin gas analysis method of the present invention can be carried out by molding each of the materials for the substrate, light-emitting layer, and other components described above into an appropriate shape, and laminating the resulting molded products together to produce a gas-reactive film composite having the structure exemplified above.

[0133] If necessary, the obtained gas-reactive film laminate may be stored in a packaging material until it is subjected to step 2. Prior to subjecting the gas-reactive film laminate to step 2, the gas-reactive film laminate may be removed from the packaging material. In addition, when the gas-reactive film laminate includes a separator, the separator may be peeled off and removed before being subjected to step 2.

[0134] <Analysis Method: Step 2> Step 2 of the skin gas analysis method of the present invention can be performed by attaching the gas reactive film multilayer to the skin using the adhesive force of the light-emitting layer or other adhesive layer.

[0135] Fig. 6 is a longitudinal sectional view schematically showing an example of a state in which the gas reactive film laminate 200 shown in Fig. 2 is subjected to step 2 of the analysis method of the present invention. In Fig. 6, the gas reactive film laminate 206 is a laminate having a configuration obtained by peeling and removing the separator 251 from the gas reactive film laminate 200 shown in Fig. 2.

[0136] In this example, gas-reactive film composite 206 is placed by adhering gas-reactive film composite 206 so that the surface on the light-emitting layer 221 side is in contact with skin 600 of the subject, and fixing gas-reactive film composite 206 on skin 600 by the adhesive force of adhesive layer 231. By placing gas-reactive film composite 206 in this manner, a sealed area is formed by substrate 111, adhesive layer 231, and skin 600, and light-emitting layer 221 and adsorbent layer 241 are positioned within this sealed area. By configuring this positional relationship, light-emitting layer 221 can effectively capture the gas to be detected that has been diffused from skin 600, thereby improving analytical performance.

[0137] The gas to be detected among the fluids diffused from the skin 600 reaches the luminescent layer 221 and reacts with the gas-reactive luminescent material in the luminescent layer 221. On the other hand, fluids that adversely affect the analysis, such as water vapor or water, are adsorbed by the adsorbent layer 241, thereby reducing the amount of moisture that adversely affects the luminescent layer 221 in step 2.

[0138] When a physical impact is applied to the surface of the composite 206 on the substrate side, the protective layer 212 absorbs the impact, thereby preventing deterioration such as scratches on the substrate 111.

[0139] Fig. 8 is a longitudinal sectional view schematically showing an example of a state in which the gas reactive film laminate 400 shown in Fig. 4 is subjected to step 2 of the analysis method of the present invention. In Fig. 8, the gas reactive film laminate 406 is a laminate having a configuration obtained by peeling and removing the separator 251 from the gas reactive film laminate 400 shown in Fig. 4.

[0140] In this example, gas-reactive film composite 406 is attached so that the surface of gas-reactive film composite 406 facing light-emitting layer 421 contacts skin 600 of the subject, and gas-reactive film composite 406 is fixed to skin 600 by the adhesive force of adhesive layer 431, thereby installing gas-reactive film composite 406. With this installation, substrate 111, frame 461, adhesive layer 431, and skin 600 form an enclosed area, part of which is occupied by light-emitting layer 421 and adsorbent layer 441, with the remainder forming void 871. With this positional relationship, the gas to be detected that has been emitted from skin 600 is stored in void 871, then captured by light-emitting layer 421, and reacts with the gas-reactive light-emitting material in light-emitting layer 421. Meanwhile, fluids that adversely affect analysis, such as water vapor or water, are stored in void 871 and then adsorbed by adsorbent layer 241. As a result, the proportion of fluid that adversely affects the analysis that is absorbed by the adsorbent layer 441 before reaching the light-emitting layer 421 can be increased.

[0141] 6, when a physical impact is applied to the surface of the composite 206 on the substrate side, the protective layer 212 absorbs the impact, thereby preventing deterioration such as scratches on the substrate 111.

[0142] <Analysis Method: Step 3> After step 2 is completed, step 3 can be performed as an optional step. In step 3, the gas-reactive luminescent material that has reacted with skin gases is sealed with a sealing substrate. By performing such sealing, it becomes possible to maintain the luminescent layer in a state in which its deterioration is suppressed. Therefore, when step 3 is performed in this manner, it becomes possible to perform an advantageous analysis when there is a long period of time between the completion of step 2 and the implementation of step 4.

[0143] FIG. 7 is a longitudinal cross-sectional view schematically illustrating an example of the state in which the gas reactive film composite 206 shown in FIG. 6 is subjected to step 3 of the analysis method of the present invention. In FIG. 7 , a sealing substrate 700 is attached to the surface of the gas reactive film composite 206 facing the light-emitting layer 221, thereby achieving sealing. In this example, the sealing substrate 700 is a film including a substrate 711 and a protective layer 712, and is attached so that the substrate 711 side contacts the gas reactive film composite 206. The substrate 711 and the protective layer 712 may be layers having the same material and thickness as the substrate 111 and the protective layer 212, respectively. By using a sealing substrate having such a configuration as the sealing substrate and performing sealing in this manner, sealing can be achieved on the sealed side to the same extent as sealing by the substrate 111 and the protective layer 212. Therefore, in the area sealed by the substrate 111, the adhesive layer 231, and the substrate 711, the light-emitting layer 221 can be maintained in a state in which its deterioration is suppressed. Therefore, when step 3 is performed in this manner, it becomes possible to carry out an advantageous analysis when the period between the end of step 2 and the implementation of step 4 is long.

[0144] FIG. 9 is a longitudinal cross-sectional view schematically illustrating an example of the state in which the gas reactive film composite 406 shown in FIG. 8 is subjected to step 3 of the analysis method of the present invention. In FIG. 9 , a sealing substrate 700 is attached to the surface of the gas reactive film composite 406 facing the adhesive layer 431 to achieve sealing. In this example, the sealing substrate 700 is the same as that shown in the example of FIG. 7 . By using a sealing substrate having such a configuration and performing sealing in this manner, sealing can be achieved on the sealed surface to the same extent as sealing by the base material 111 and protective layer 212. Therefore, in the area sealed by the base material 111, frame 461, adhesive layer 431, and base material 711, a sealed area is formed, with the light-emitting layer 421 and adsorbent layer 441 occupying a portion of the interior, and the remainder being a void 971. In this area, the light-emitting layer 421 can be maintained in a state in which its deterioration is suppressed. Therefore, when step 3 is performed in this manner, it becomes possible to carry out an advantageous analysis when the period between the end of step 2 and the implementation of step 4 is long.

[0145] <Analysis Method: Step 4> In Step 4, the gas-reactive film composite after Step 2 is subjected to irradiation with excitation light, either directly or after Step 3, and the fluorescence or phosphorescence emitted from the gas-reactive luminescent material in the luminescent layer is detected using a detector.

[0146] Irradiation with excitation light can be performed using a light source that emits excitation light of a desired wavelength, and detection of fluorescence or phosphorescence can be performed using known devices, such as a combination of a camera capable of detecting light of the fluorescence or phosphorescence wavelength and an image analysis device.

[0147] Irradiation with excitation light and detection by a detector can be performed from either the substrate side of the gas-reactive film composite (in the examples of Figures 7 and 9, the side facing the substrate 111 and protective layer 212) or the side opposite the substrate (in the examples of Figures 7 and 9, the side facing the sealing substrate 700).

[0148] 7 and 9, the sealing substrate is made of the same material and thickness as the substrate 111 and the protective layer 212, respectively. Therefore, irradiation with excitation light and detection with a detector can be performed from either the substrate side or the opposite side of the gas reactive film multilayer. For example, irradiation with excitation light may be performed from the substrate side and detection with a detector may be performed from the substrate side, irradiation with excitation light may be performed from the substrate side and detection with a detector may be performed from the opposite side of the substrate, irradiation with excitation light may be performed from the opposite side of the substrate and detection with a detector may be performed from the substrate side, or irradiation with excitation light may be performed from the opposite side of the substrate and detection with a detector may be performed from the opposite side of the substrate. Of these embodiments, an embodiment advantageous for implementing step 4 can be appropriately selected and implemented.

[0149] When the gas reactive film composite to be subjected to step 4 has a protective layer provided on a substrate, the protective layer may be left as is without being peeled off when performing step 4 if it does not interfere with step 4. Alternatively, when the protective layer interferes with step 4 when performing step 4, the protective layer may be peeled off and the remaining part of the gas reactive film composite may be subjected to step 4. For example, in the examples of Figures 7 and 9, protective layer 212 and protective layer 712 may be left as is without being peeled off when performing step 4, or one or both of them may be peeled off before performing step 4.

[0150] Depending on the type of light-emitting layer used and the gas to be detected, it may be preferable to use a sealing substrate with optical properties different from those of the light-transmitting sealing substrate 700 shown in Figures 7 and 9. For example, a light-absorbing sealing substrate having the property of absorbing incident light, such as a black film, can be used, or a light-reflective sealing substrate having the property of reflecting incident light, such as a reflector, can also be used. When a light-absorbing or light-reflective sealing substrate is used, irradiation with excitation light and detection by a detector can be performed from the surface on the substrate side.

[0151] When the gas-reactive film composite is subjected to step 4 without going through step 3, the gas-reactive film composite may be peeled off from the surface of the subject to be analyzed before being subjected to step 4, or step 4 may be performed without peeling off from the surface of the subject to be analyzed. For example, excitation light may be irradiated from the substrate-side surface of the gas-reactive film composite that remains attached to the skin of the living body to be analyzed, and fluorescence or phosphorescence may be detected by a detector. Such detection may be performed continuously, and the amount of gas emitted from the skin may be measured over time.

[0152] <Application of analytical method> The gas-reactive film multilayer of the present invention and the analytical method of the present invention using the same can be used for qualitative or quantitative analysis of the emission of various skin gases from the skin of humans and non-human animals. As described above in the explanation of the light-emitting layer, by appropriately selecting the light-emitting material, various skin gases can be detected, and various biological information corresponding to the emission of these skin gases can be obtained non-invasively and easily.

[0153] 111, 711 Substrate 100, 200, 206, 300, 400, 406, 500 Gas reactive film composite 111D, 111U, 121D, 221D, 431D Surface 121, 221, 421 Light emitting layer 212, 712 Protective layer 231, 431 Adhesive layer 241, 441 Adsorbent layer 251 Separator 313 Substrate with ventilation hole 314 Ventilation hole 461 Frame 471, 472D, 472U, 871, 971 Gap 481 Support substrate 482 Hole 600 Skin 700 Sealing substrate

Claims

1. A light-emitting device comprising a substrate made of resin and a light-emitting layer containing a gas-reactive light-emitting material, the moisture permeability of the substrate being 7 g / m ２ Gas reactive film laminates that are less than 24 hours old.

2. The gas reactive film composite according to claim 1, wherein the average light transmittance of said substrate in the wavelength range of 300 to 400 nm is 80% or more.

3. The gas reactive film multilayer according to claim 1, wherein the base material has an average light transmittance of 85% or more in the wavelength range of 400 to 750 nm.

4. The gas reactive film composite according to claim 2, wherein the base material has an average light transmittance of 85% or more in the wavelength range of 400 to 750 nm.

5. The gas reactive film composite of claim 1, wherein said gas reactive luminescent material is a material that reacts with skin gases.

6. The gas reactive film composite according to claim 1, wherein said gas reactive luminescent material is a material whose photoluminescent properties change upon reaction with a gas.

7. The gas reactive film composite according to claim 1, wherein said resin contains a polymer containing an alicyclic structure.

8. The gas reactive film composite according to claim 7, wherein the polymer having an alicyclic structure is a norbornene-based polymer; and the norbornene-based polymer comprises at least one selected from the group consisting of a hydrogenated ring-opening polymer of a monomer having a norbornene structure, an addition copolymer of a monomer having a norbornene structure and an α-olefin, and a hydrogenated copolymer thereof.

9. The gas-reactive film composite according to claim 7, wherein the alicyclic structure-containing polymer is a hydrogenated block copolymer [E]; and the hydrogenated block copolymer [E] is a hydrogenated block copolymer obtained by hydrogenating a block copolymer [D] consisting of a polymer block [A] mainly composed of a repeating unit [I] derived from an aromatic vinyl compound, and a polymer block [B] mainly composed of a repeating unit [I] derived from an aromatic vinyl compound and a repeating unit [II] derived from a linear conjugated diene compound, or a polymer block [C] mainly composed of a repeating unit [II] derived from a linear conjugated diene compound.

10. The gas reactive film composite of claim 1, further comprising a protective layer disposed on the substrate opposite the light emitting layer.

11. The gas reactive film composite of claim 1, further comprising a peelable sealing layer disposed on the surface of said light emitting layer opposite said substrate.

12. A skin gas analysis method comprising: step 1 of preparing a gas-reactive film composite according to any one of claims 1 to 11; step 2 of placing the gas-reactive film composite on the skin of a subject and causing skin gas to react with the gas-reactive luminescent material in the gas-reactive film composite; and step 4 of irradiating the gas-reactive luminescent material with excitation light and detecting fluorescence or phosphorescence emitted from the gas-reactive luminescent material.

13. The skin gas analysis method according to claim 12, further comprising step 3, after step 2 and before step 4, of sealing the gas-reactive luminescent material to which the skin gas has reacted with a sealing substrate.

14. The method for analyzing skin gases according to claim 13, wherein the sealing substrate is made of a resin containing a polymer having an alicyclic structure.

15. The method for analyzing skin gases according to claim 13, wherein the sealing substrate is a black film.

16. The method for analyzing skin gases according to claim 13, wherein the sealing substrate is a reflector.

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