JP2023024453A - Diaper mounted with enzyme battery and system - Google Patents
Diaper mounted with enzyme battery and system Download PDFInfo
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- JP2023024453A JP2023024453A JP2022186268A JP2022186268A JP2023024453A JP 2023024453 A JP2023024453 A JP 2023024453A JP 2022186268 A JP2022186268 A JP 2022186268A JP 2022186268 A JP2022186268 A JP 2022186268A JP 2023024453 A JP2023024453 A JP 2023024453A
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
Description
本発明は、酵素電池が搭載されたおむつ並びにシステムに関する。 TECHNICAL FIELD The present invention relates to a diaper and system equipped with an enzyme battery.
少子高齢社会化による医療費増大や労働力不足などが問題となっている。特に介護現場においては、慢性的な人手不足が問題となり労働環境の改善が急務となっている。
介護作業の中でも、寝たきり患者や高齢者などに対する排泄ケアは介護者に体力的・精神的に過大な負担を負わせている。
通常、介護施設や病院などでは、排泄があった状態で患者を長時間放置することや、おむつ漏れによるシーツやベッドの汚染を防ぐため、定期的におむつの汚れ具合を確認し、おむつ交換がなされている。しかし、この確認作業には、排泄をしていない場合や、交換する必要がない場合も多分に含まれ、本来不必要なおむつ開閉作業や交換する必要のないおむつ交換作業が発生し、介護者への負担を大きくしている。
排尿の有無をセンサーなどによって検知し、排泄有無をおむつの確認無しに知る事ができれば、不必要なおむつ開閉及び交換作業を軽減させることが可能となる。
With the declining birthrate and aging population, rising medical costs and labor shortages are becoming issues. Especially in nursing care sites, there is an urgent need to improve the working environment due to chronic labor shortages.
Among nursing care tasks, continence care for bedridden patients and elderly people imposes an excessive physical and mental burden on caregivers.
Usually, in nursing care facilities and hospitals, it is necessary to regularly check the dirtiness of diapers and change diapers to prevent patients from being left for a long time after excretion and to prevent sheets and beds from being contaminated by diaper leakage. is done. However, this confirmation work often includes cases where the diaper has not been excreted or when there is no need to change diapers. increasing the burden on
If the presence or absence of urination can be detected by a sensor or the like and the presence or absence of urination can be known without checking the diaper, unnecessary diaper opening/closing and changing operations can be reduced.
改善策として、おむつ内側表面に水分センサーを設置し排尿を検知する方法が報告されている（特許文献１、２）。しかし、従来の水分センサーは駆動に電源を別に必要とするため、電池交換の手間や配線の問題、また、センサーに金属電極が使用される場合では、廃棄の際の分別の手間などが問題となる。
As a remedy, a method has been reported in which a moisture sensor is installed on the inner surface of the diaper to detect urination (
本発明の目的は、酵素電池が搭載されたおむつにより、電池交換の手間がなく、容易に廃棄が可能な排尿を検知するセンサーの電源及び、センサーを提供することである。 SUMMARY OF THE INVENTION An object of the present invention is to provide a power supply for a sensor that detects urination and a sensor that can be easily discarded without the need for battery replacement, using a diaper equipped with an enzyme battery.
本発明者らは、前記課題を解決すべく検討を重ねた結果、本発明に至った。
すなわち本発明は、構成部材として少なくともトップシート、吸水材、およびバックシートを含むおむつであって、前記トップシートと前記バックシートとの間に酵素電池が位置され、
前記酵素電池は、正極および、負極を含んでなり、
前記正極または前記負極の少なくとも一方が酵素を含むことを特徴とする酵素電池が搭載されたおむつに関する。
The present inventors have reached the present invention as a result of repeated studies to solve the above problems.
That is, the present invention provides a diaper comprising at least a top sheet, a water absorbent material, and a back sheet as constituent members, wherein an enzyme battery is positioned between the top sheet and the back sheet,
The enzyme battery comprises a positive electrode and a negative electrode,
The present invention relates to a diaper equipped with an enzyme battery, wherein at least one of the positive electrode and the negative electrode contains an enzyme.
また、本発明は、前記酵素電池が、トップシートと吸水材との間に位置する上記おむつに関する。 The present invention also relates to the above diaper, wherein the enzyme battery is positioned between the top sheet and the absorbent material.
また、本発明は、前記酵素電池が、吸水材の内部に位置する上記おむつに関する。 The present invention also relates to the diaper, wherein the enzyme battery is located inside the water absorbent material.
また、本発明は、前記酵素電池が、吸水材とバックシートとの間に位置する上記おむつに関する。 The present invention also relates to the diaper, wherein the enzyme battery is positioned between the water absorbent material and the backsheet.
また、本発明は、酵素電池が、おむつの外部より供給された尿中の成分により発電しうる酵素を含有する上記おむつに関する。 The present invention also relates to the above diaper, wherein the enzyme battery contains an enzyme capable of generating electricity from urine components supplied from the outside of the diaper.
また、本発明は、さらに、酵素電池の内部または近傍に燃料を含有する上記おむつに関する。 In addition, the present invention further relates to the above diaper containing a fuel inside or near the enzyme battery.
また、本発明は、尿中に含まれる1種類以上の有機物により発電しうる酵素を含有す
る上記おむつに関する。
The present invention also relates to the above diaper containing an enzyme capable of generating electricity from one or more organic substances contained in urine.
また、本発明は、上記おむつを使用して、燃料の残存量と発電量とから排尿量を演算する手段を備えるシステムに関する。 The present invention also relates to a system comprising means for calculating the amount of urination from the remaining amount of fuel and the amount of power generated using the diaper.
また、本発明は、上記おむつを使用し、酵素電池の発電量から、尿中に含まれる1種類
以上の有機物の濃度を演算する手段を備えるシステムに関する。
The present invention also relates to a system that uses the above diaper and has means for calculating the concentration of one or more organic substances contained in urine from the amount of power generated by the enzyme battery.
また、本発明は、上記おむつを使用し、排尿による酵素電池の発電量の変化から、排尿回数を演算する手段を備えるシステムに関する。 The present invention also relates to a system that uses the above diaper and has means for calculating the number of times of urination from changes in the amount of power generated by the enzyme battery due to urination.
また、本発明は、さらに、酵素電池の発電に連動する外部伝達手段を備える上記システムに関する。 Moreover, the present invention further relates to the above system comprising an external transmission means interlocked with the power generation of the enzyme battery.
本発明の酵素電池を搭載したおむつを用いることにより、電池交換の手間がなく、容易に廃棄が可能な排尿を検知するセンサーの電源及び、センサーが実現可能となる。 By using the diaper equipped with the enzyme battery of the present invention, it is possible to realize a power source and a sensor for detecting urination that can be easily discarded without the need for battery replacement.
以下、詳細に本発明について説明する。 The present invention will be described in detail below.
＜酵素電池を搭載したおむつ（トップシート、吸水材、バックシート）＞
本発明におけるおむつは、少なくとも、トップシート、吸水材、バックシートを含むものである。トップシートは、肌に直接接し、おむつの最も内側（肌側）を構成する部分で、不織布（ポリプロピレン、ポリエステル、レーヨンなど）や綿などからなり、排泄された尿を速やかに拡散、浸透し、吸水材に送る役割を担う。
吸水材は、綿状パルプ、高分子吸水剤、給水紙などからなり、トップシートから流入した尿を吸水、保水する役割を担う。バックシートは、ポリエチレンフィルムなどからなり、防水機能を有し、尿などの漏れを防止する役割を担う。
<Diaper equipped with an enzyme battery (top sheet, absorbent material, back sheet)>
A diaper in the present invention includes at least a top sheet, a water absorbing material, and a back sheet. The top sheet is the innermost part (skin side) of the diaper that comes into direct contact with the skin. Plays the role of sending to the water absorbing material.
The water-absorbing material is composed of cotton-like pulp, a polymer water-absorbing agent, water-retaining paper, and the like, and plays a role of absorbing and retaining urine that has flowed in from the top sheet. The back sheet is made of polyethylene film or the like, has a waterproof function, and plays a role in preventing leakage of urine and the like.
酵素電池をおむつに搭載する場合は、トップシートと吸水材とバックシートとを順に有し、酵素電池がトップシートとバックシートの間にある。つまり、トップシートと吸水材の間、吸水材の内部、および吸水材とバックシートの間のいずれかの位置で搭載される。酵素電池がトップシートの内側に搭載されていることは、安定駆動に必要な酵素電池内部への尿の十分な浸透において重要な意味をなす。トップシートの内側にある場合、親水的材料からなるトップシートや、吸水材から酵素電池へ尿が拡散、浸透されるため、酵素電池がトップシートの外側に露出している場合に比べ、酵素電池内へ尿を効果的に供給することが可能となる。また、トップシートの外側に露出していないため、酵素電池が肌に直接触れることを防ぎ、かぶれや、酵素電池の破損などを防止できる。 When the enzyme battery is mounted on a diaper, the diaper has a top sheet, a water absorbent material and a back sheet in that order, and the enzyme battery is between the top sheet and the back sheet. That is, it is mounted at any position between the topsheet and the absorbent material, inside the absorbent material, or between the absorbent material and the backsheet. The fact that the enzyme battery is mounted inside the top sheet is significant in terms of sufficient penetration of urine into the enzyme battery, which is necessary for stable operation. When the enzyme battery is inside the top sheet, urine diffuses and permeates from the top sheet made of a hydrophilic material or the water-absorbing material into the enzyme battery. It becomes possible to effectively supply urine to the inside. In addition, since it is not exposed to the outside of the top sheet, it is possible to prevent the enzyme battery from coming into direct contact with the skin, thereby preventing rashes and breakage of the enzyme battery.
＜酵素電池＞
酵素電池は、酵素が、糖やアルコール、有機酸等の多様な有機物を酸化し、アノード（負極）で電子及びイオンを発生させ、カソード（正極）側で酸素還元反応させることにより発電しうる発電デバイスである。
電源としての利用の外に、発電の有無や発電量を検知することにより、燃料となる有機物等を対象としたセンサーとして利用することも可能となる。
更に、酵素反応により発電した電力を用いて、同センサーを駆動させることにより、外部から電力供給不要な電源フリーのセンサーとして利用することが出来る。
尿中に含まれる有機物や水などの成分により起きる発電は、２通りがある。一つは、有機物が燃料として発電する場合であり、もう一つは、予め酵素電池の内部または近傍に燃料が位置され、尿中の水により、当該燃料が移動し、酵素と反応して発電する場合である。
すなわち、尿中や尿糖、尿酸等の有機物を燃料及び／又はセンシング対象物として利用される。また、尿などの外部より供給される生体試料中に燃料として利用できる有機物を含まなくても、予め燃料となる有機物をおむつに内蔵することで、外部より供給された水分などの液体成分により、当該燃料が運ばれ、酵素と反応して発電することもできる。このように、本発明では酵素電池は電源としての利用と、センサーとしての利用、およびその両方としての利用が出来る。
酵素電池の構成としては、燃料を酸化するアノードと、酸素還元が起こるカソードと、アノードとカソードを分離するセパレータを含む。但し、アノードとカソードを電気的に分離することができればセパレータは必ずしもなくても構わない。また、アノードからカソード側にイオンを伝達するためのイオン伝導体を含んでいても良い。小型・軽量化や保存安定性等を考慮すると、燃料及び／又はセンシング対象物である尿中に含まれる電解質を使用する形態の酵素電池の方が好ましい場合がある。
アノードとカソードが完全に分離していない、非セパレータ系や紙等をセパレータに使用する形態の酵素電池においては、燃料等に含まれる不純物成分がカソード反応の酸素還元触媒を被毒する場合があり、活性低下、出力不安定化が生じやすいため注意が必要となる。特に白金等の貴金属触媒は被毒されやすいため同系においての使用は好ましくない場合がある。一方、貴金属を含まない酵素電池用炭素触媒はこれら貴金属触媒よりも被毒に強いため、不純物が存在する系においても好適に使用できる。
加えて、不織布やフェルト、紙など易廃棄なセパレータに直接アノード及びカソードを塗布し作製されるデバイスに対して、本発明に用いられる酵素電池用炭素触媒をカソードに使用すると、高価な貴金属や酸素還元酵素を使用せず低コストで、使い捨て可能（易廃棄、リサイクル不要など）なデバイスを実現することが可能となる。
<Enzyme battery>
Enzyme batteries generate electricity by oxidizing various organic substances such as sugars, alcohols, and organic acids using enzymes, generating electrons and ions at the anode (negative electrode), and causing an oxygen reduction reaction at the cathode (positive electrode). Device.
In addition to being used as a power source, by detecting the presence or absence of power generation and the amount of power generated, it can also be used as a sensor for organic matter that is used as fuel.
Furthermore, by driving the sensor using the power generated by the enzymatic reaction, it can be used as a power-free sensor that does not require power supply from the outside.
There are two types of power generation caused by components such as organic matter and water contained in urine. One is the case where organic matter is used as fuel to generate electricity, and the other is when fuel is placed in advance in or near the enzyme cell, and water in the urine moves the fuel and reacts with the enzyme to generate electricity. is the case.
In other words, organic substances such as urine, urinary sugar, and uric acid are used as fuel and/or objects to be sensed. In addition, even if an externally supplied biological sample such as urine does not contain an organic substance that can be used as a fuel, by incorporating an organic substance that can be used as a fuel into the diaper in advance, liquid components such as water supplied from the outside can The fuel can also be transported and reacted with enzymes to generate electricity. Thus, in the present invention, the enzyme battery can be used as a power source, as a sensor, or as both.
The structure of an enzyme cell includes an anode for oxidizing fuel, a cathode for oxygen reduction, and a separator for separating the anode and cathode. However, if the anode and cathode can be electrically separated, the separator may not necessarily be provided. It may also contain an ionic conductor for transmitting ions from the anode to the cathode side. In consideration of downsizing, weight reduction, storage stability, and the like, an enzyme battery that uses fuel and/or electrolytes contained in urine, which is a sensing target, may be preferable.
In the case of an enzyme cell in which the anode and cathode are not completely separated, and in which a non-separator type or paper is used as a separator, impurities contained in the fuel may poison the oxygen reduction catalyst of the cathode reaction. , activity decrease, and output instability are likely to occur, so caution is required. In particular, noble metal catalysts such as platinum are susceptible to poisoning, so their use in the same system may not be preferred. On the other hand, carbon catalysts for enzyme cells that do not contain noble metals are more resistant to poisoning than these noble metal catalysts, so they can be suitably used even in systems where impurities are present.
In addition, when the carbon catalyst for an enzyme battery used in the present invention is used as a cathode for a device manufactured by directly applying an anode and a cathode to easily disposed separators such as non-woven fabric, felt, and paper, expensive precious metals and oxygen are used. It is possible to realize a low-cost, disposable (easy-to-dispose, no-recycling, etc.) device without using a reductase.
＜回路配線＞
回路配線とは、酵素電池において正極および負極と外部デバイスを電気的に接続し、回路を形成するための導電性部材である。回路配線は、正極あるいは負極と別途用意された導電性部材を接続し更に外部デバイスに接続してもよく、正極あるいは負極の導電性支持体をそのまま延長して回路配線として外部デバイスと接続してもよい。回路配線と外部デ
バイスを接続する方法としては特に限定するものではなく、接着剤あるいは粘着剤による接続の他に、スナップボタン、マグネット、クリップ、ファスナー、マジックテープ（登録商標）等を用いた接続が例示できる。
回路配線の材料としては、導電性を有する非金属材料であれば特に限定するものではない。例えば、カーボンペーパーやカーボンクロス、カーボンフェルト等の導電性炭素材料の他、紙類、布類等の非導電性支持体に酵素電池回路配線用導電炭素組成物やポリアニリン、ポリアセチレン、ポリピロール、ポリチオフェン等の導電性高分子を塗布、乾燥したものやそれらを併用したものを用いてもよい。廃棄の容易さやコストの観点から非導電性支持体に酵素電池回路配線用導電炭素組成物を塗布、乾燥したものを用いた方が好ましい。特に非導電性支持体は折り曲げ可能な支持体であることが好ましい。更には、紙類の非導電性支持体に酵素電池回路配線用導電炭素組成物を塗布、乾燥したものを用いた方が好ましい。
<Circuit wiring>
The circuit wiring is a conductive member for electrically connecting the positive and negative electrodes and an external device in an enzyme battery to form a circuit. The circuit wiring may connect the positive electrode or the negative electrode to a separately prepared conductive member and then connect to an external device, or the conductive support of the positive electrode or the negative electrode may be extended as it is and connected to the external device as circuit wiring. good too. The method of connecting the circuit wiring and the external device is not particularly limited, and in addition to connection using adhesives or adhesives, connection using snap buttons, magnets, clips, fasteners, Velcro (registered trademark), etc. is possible. I can give an example.
The material for the circuit wiring is not particularly limited as long as it is a non-metallic material having conductivity. For example, in addition to conductive carbon materials such as carbon paper, carbon cloth, and carbon felt, conductive carbon compositions for enzyme cell circuit wiring, polyaniline, polyacetylene, polypyrrole, polythiophene, etc. are applied to non-conductive supports such as papers and cloths. may be applied and dried, or a combination of these may be used. From the viewpoints of ease of disposal and cost, it is preferable to apply the conductive carbon composition for enzyme cell circuit wiring to a non-conductive support and then use a dried one. In particular, the non-conductive support is preferably a bendable support. Furthermore, it is preferable to apply the conductive carbon composition for circuit wiring of an enzyme cell to a non-conductive support such as paper, and then use a dried one.
＜酵素電池回路配線用導電炭素組成物＞
酵素電池回路配線用導電炭素組成物は、少なくとも黒鉛やカーボンブラック、グラフェン系材料などの導電性炭素と、溶剤とバインダーを含む。また、酵素電池回路配線用導電炭素組成物は、必要に応じて分散剤、増粘剤、成膜助剤、消泡剤、レベリング剤、防腐剤、ｐＨ調整剤等を配合できる。導電性炭素及び溶剤とバインダー、分散剤の割合は、特に限定されるものではなく、広い範囲内で適宜選択され得る。ＶＯＣ排出の観点から、水あるいは水性溶剤を用いることが好ましく、それに伴いバインダーおよび分散剤等も水性であることが好ましい。
<Conductive carbon composition for enzyme battery circuit wiring>
The conductive carbon composition for enzyme battery circuit wiring contains at least conductive carbon such as graphite, carbon black, and graphene-based material, a solvent, and a binder. In addition, the conductive carbon composition for enzyme cell circuit wiring may optionally contain a dispersant, a thickener, a film forming aid, an antifoaming agent, a leveling agent, an antiseptic, a pH adjuster, and the like. The ratio of conductive carbon and solvent to binder and dispersant is not particularly limited and can be appropriately selected within a wide range. From the viewpoint of VOC emission, it is preferable to use water or an aqueous solvent, and along with that, it is preferable that the binder, dispersant, etc. are also aqueous.
＜導電性支持体＞
酵素電池において、正極および負極に導電性支持体を用いても良い。酵素電池に用いる導電性支持体は、導電性を有する材料であれば特に限定は無い。カーボンペーパーやカーボンクロス等導電性の炭素材料からなる導電層や金属箔、金属メッシュ等が挙げられる。また、回路配線と同様に、紙類、布類等の非導電性支持体に酵素電池回路配線用導電炭素組成物やポリアニリン、ポリアセチレン、ポリピロール、ポリチオフェン等の導電性高分子を塗布、乾燥したものやそれらを併用したものを用いてもよい。前記組成物の塗布方法としては、特に限定されるものではなく、酵素電池用回路配線の作製の際に使用するような一般的な方法を適用できる。
廃棄の容易さやコストの観点から、非導電性支持体に酵素電池回路配線用導電炭素組成物を塗布、乾燥したものを用いた方が好ましい。特に非導電性支持体は折り曲げ可能な支持体であることが好ましい。更に、紙類の非導電性支持体に酵素電池回路配線用導電炭素組成物を塗布、乾燥したものを用いた方が好ましい。
<Conductive support>
In an enzyme battery, a conductive support may be used for the positive electrode and the negative electrode. The conductive support used in the enzyme battery is not particularly limited as long as it is a conductive material. A conductive layer made of a conductive carbon material such as carbon paper or carbon cloth, a metal foil, a metal mesh, or the like can be used. In the same manner as the circuit wiring, a non-conductive support such as paper or cloth may be coated with a conductive carbon composition for enzyme cell circuit wiring or a conductive polymer such as polyaniline, polyacetylene, polypyrrole or polythiophene, and dried. or a combination thereof may be used. A method for applying the composition is not particularly limited, and a general method used for producing circuit wiring for an enzyme battery can be applied.
From the viewpoints of ease of disposal and cost, it is preferable to apply the conductive carbon composition for enzyme cell circuit wiring to a non-conductive support and then use the dried one. In particular, the non-conductive support is preferably a bendable support. Furthermore, it is preferable to apply the conductive carbon composition for circuit wiring of an enzyme cell to a non-conductive support such as paper, and then use a dried one.
＜酵素電池用負極＞
酵素電池用負極では、燃料の酸化反応により発生した電子をカソードに供給する。酵素電池用負極は、導電性支持体やセパレータ等の基材に前記酵素電池回路配線用導電炭素組成物や、導電性炭素材料や酵素電池用炭素触媒などのペーストを直接塗布し乾燥した塗膜や、転写基材などに前記酵素電池回路配線用導電炭素組成物を塗布し乾燥することにより形成された塗膜を支持体やセパレータ等に転写して作製した塗膜に酵素やメディエータを担持させたり、導電性支持体に酵素やメディエータを直接担持させたり、酵素を含む酵素電池回路配線用導電炭素組成物を支持体に塗布し乾燥したりして作製される。
前記組成物の塗布方法としては、特に限定されるものではなく、酵素電池用回路配線の作製の際に使用するような一般的な方法を適用できる。
酵素やメディエータを担持する方法は、上記組成物に含ませて行っても良いし、塗布後乾燥した塗膜や、導電性支持体に後から行っても良い。後から行う場合では、酵素やメディエータを溶解させた液を上記塗膜や、導電性支持体に浸漬等させた後、乾燥させて担持する方法等が使用できる。
<Negative electrode for enzyme battery>
In the negative electrode for an enzyme battery, electrons generated by the oxidation reaction of the fuel are supplied to the cathode. The negative electrode for an enzyme battery is a coated film obtained by directly applying a paste such as the conductive carbon composition for circuit wiring of an enzyme battery, a conductive carbon material, or a carbon catalyst for an enzyme battery to a base material such as a conductive support or a separator and drying the paste. Alternatively, the coating film formed by applying the conductive carbon composition for enzyme battery circuit wiring to a transfer base material and drying is transferred to a support, separator, etc., and the enzyme or mediator is supported on the coating film. Alternatively, an enzyme or mediator may be directly supported on a conductive support, or a conductive carbon composition for enzyme cell circuit wiring containing an enzyme may be coated on a support and dried.
A method for applying the composition is not particularly limited, and a general method used for producing circuit wiring for an enzyme battery can be applied.
The method of supporting the enzyme or mediator may be carried out by including it in the above composition, or may be carried out later on the coating film dried after coating or on the conductive support. In the case of carrying out afterward, a method of immersing a liquid in which an enzyme or a mediator is dissolved in the coating film or the conductive support, followed by drying and carrying the solution can be used.
＜酵素電池負極用酵素＞
本発明における酵素としては、反応により電子を授受できる酵素であれば特に制限はなく、供給する燃料やコスト、デバイスの種類等に応じて適宜選択される。酵素としては、物質代謝など生体内での多くの酸化還元反応を触媒する酸化還元酵素が好ましい。
酵素電池の負極に用いる酵素は電子を放出できるものであればよく、糖や有機酸などのオキシダーゼやデヒドロゲナーゼなどが利用できる。中でも、他の酵素に比べ安価で、安定性が高く、人体の血液や尿などの生体試料に含まれるグルコースを燃料にできるグルコースオキシダーゼやグルコースデヒドロゲナーゼが好ましい場合がある。
<Enzyme Battery Anode Enzymes>
The enzyme in the present invention is not particularly limited as long as it can give and receive electrons by reaction, and is appropriately selected according to the fuel to be supplied, the cost, the type of device, and the like. The enzyme is preferably an oxidoreductase that catalyzes many redox reactions in vivo such as substance metabolism.
Any enzyme can be used as the negative electrode of the enzyme battery as long as it can release electrons, and oxidases such as sugars and organic acids, dehydrogenases, and the like can be used. Among them, glucose oxidase and glucose dehydrogenase, which are less expensive than other enzymes, have high stability, and can use glucose contained in biological samples such as human blood and urine as fuel, may be preferable.
＜メディエータ＞
酵素の種類によって、電極に直接電子を伝達できる直接電子移動型（ＤＥＴ型）酵素と直接電子を伝達できない酵素が存在する。ＤＥＴ型以外の酵素は、燃料の酸化によって生じた電子を酵素から電極（アノード）に伝達するまたは、アノードから受け取った電子を電極（カソード）から酵素に伝達する役割を担うメディエータと併用することが好ましい。メディエータとしては、電極と電子の授受ができる酸化還元物質であれば特に制限はなく、従来公知のものを使用できる。
メディエータの使用方法としては、電極に担持させる方法や電解液に溶解させて使用する方法等がある。メディエータとしては、テトラチアフルバレン、ハイドロキノンや１，４‐ナフトキノン等のキノン類、フェロセン、フェリシアン化物、オスミウム錯体、及びこれら化合物を修飾したポリマー等が例示できる。分別、廃棄の観点から非金属化合物が好ましい。
<Mediator>
Depending on the types of enzymes, there are direct electron transfer (DET) enzymes that can directly transfer electrons to an electrode and enzymes that cannot directly transfer electrons. Enzymes other than the DET type can be used in combination with a mediator responsible for transferring electrons generated by fuel oxidation from the enzyme to the electrode (anode) or transferring electrons received from the anode from the electrode (cathode) to the enzyme. preferable. The mediator is not particularly limited as long as it is a redox substance capable of giving and receiving electrons to and from the electrode, and conventionally known mediators can be used.
Methods of using the mediator include a method of supporting it on an electrode, a method of dissolving it in an electrolytic solution, and the like. Examples of mediators include tetrathiafulvalene, quinones such as hydroquinone and 1,4-naphthoquinone, ferrocene, ferricyanide, osmium complexes, and polymers modified with these compounds. Non-metallic compounds are preferred from the standpoint of separation and disposal.
＜酵素電池用正極＞
酵素電池用正極では、アノードで発生した電子を受け取り、電極中の還元反応によりこれを消費する。酵素電池用正極の構造としては、例えば、酸素を電子受容体として使用する酸素還元反応の場合では、反応場となる正極触媒の活性点まで電子及びプロトンの伝導パスや酸素の供給パスが確保されていることが効率的な発電を行う上では好ましい。 酵素電池用正極は、触媒に無機化合物を用いるものと酵素を用いるものがある。導電性支持体（カーボンペーパーや導電性カーボン層など）やセパレータ等の基材に正極触媒を含む組成物を直接塗布し乾燥することにより作製する方法や、転写基材などに前記組成物を塗布し乾燥することにより形成された塗膜を前記導電性支持体やセパレータ等に転写する方法等で作製される。また、正極触媒に酵素を用いるものは、酵素電池用負極と同様の方法で組成物作製、塗布を行ってもよい。
組成物の塗布方法としては、特に限定されるものではなく、例えば、ナイフコーター、バーコーター、ブレードコーター、スプレー、ディップコーター、スピンコーター、ロールコーター、ダイコーター、カーテンコーター、スクリーン印刷等の一般的な方法を適用できる。
<Positive electrode for enzyme battery>
A positive electrode for an enzyme battery receives electrons generated at the anode and consumes them through a reduction reaction in the electrode. As for the structure of the positive electrode for an enzyme battery, for example, in the case of an oxygen reduction reaction using oxygen as an electron acceptor, a conduction path for electrons and protons and a supply path for oxygen are secured to the active point of the positive electrode catalyst, which is the reaction site. It is preferable in terms of efficient power generation. Positive electrodes for enzyme batteries include those using an inorganic compound as a catalyst and those using an enzyme. A method of directly applying a composition containing a positive electrode catalyst to a base material such as a conductive support (carbon paper, a conductive carbon layer, etc.) or a separator and drying it, or applying the composition to a transfer base material. It is prepared by a method of transferring a coating film formed by drying to the above-described conductive support, separator, or the like. In addition, when an enzyme is used as a positive electrode catalyst, the composition may be prepared and applied in the same manner as the negative electrode for an enzyme battery.
The method of applying the composition is not particularly limited. method can be applied.
＜酵素電池正極用触媒＞
酵素電池正極で無機化合物を触媒として用いる場合、酸素還元触媒として貴金属触媒、卑金属酸化物触媒、酵素電池用炭素触媒などが挙げられる。コストの面などから炭素触媒が好ましい。
貴金属触媒とは、遷移金属元素のうちルテニウム、ロジウム、パラジウム、銀、オスミウム、イリジウム、白金、金から選択される元素を一種以上含む触媒である。これら貴金属触媒は単体でも別の元素や化合物に担持されたものでも良い。
卑金属酸化物触媒は、ジルコニウム、タンタル、チタン、ニオブ、バナジウム、鉄、マンガン、コバルト、ニッケル、銅、亜鉛、クロム、タングステン、およびモリブデンからなる群より選択された少なくとも１種の卑金属元素を含む酸化物を使用することができ、より好ましくはこれら卑金属元素の炭窒化物や、これら遷移金属元素の炭窒酸化物を使用
することができる。
酵素電池用炭素触媒（以下、単に炭素触媒ともいう）とは、炭素元素を基本骨格とした炭素材料からなり、それらの構成単位間に物理的・化学的な相互作用（結合）を有し、異種元素、たとえばＮ、Ｂ、Ｐなどのヘテロ原子を含み、更に場合によって卑金属元素が含まれ酸素還元活性を有する触媒材料である。ここでいう卑金属元素とは、遷移金属元素のうち貴金属元素（ルテニウム、ロジウム、パラジウム、銀、オスミウム、イリジウム、白金、金）を除く金属元素であり、卑金属元素としては、コバルト、鉄、ニッケル、マンガン、銅、チタン、バナジウム、クロム、亜鉛、およびスズからなる群より選ばれる一種以上を含有することが好ましい。
ヘテロ元素と卑金属元素を含有することは、酸素還元活性を有する上で重要な意味をなす。酵素電池用炭素触媒は、その触媒活性点として、例えば、炭素材料の基本骨格を構成する炭素の六角網面のエッジ部に導入された窒素原子やその近傍の炭素原子、また触媒表面上に卑金属元素を中心に４個の窒素が平面上に並んだ卑金属－Ｎ４構造における窒素原子や卑金属原子などが挙げられる。
酵素電池用炭素触媒は、１種または２種以上の、炭素材料と、窒素元素および／または前記卑金属元素を含有する化合物とを混合し、熱処理を行い作製された炭素触媒であって、従来公知のものを使用できる。炭素触媒に用いられる炭素材料は、無機材料由来の炭素粒子および／または有機材料を熱処理して得られる炭素粒子であれば特に限定されない。
また、酵素を触媒として用いる場合、酵素電池の正極では電子を消費できる酵素であれば良く、ビリルビンオキシダーゼ、ラッカーゼ、アスコルビン酸オキシダーゼなどの還元酵素の一種で、分子状酸素の還元を触媒する酸素還元酵素を用いることが出来る。酸素還元酵素を使用する酵素電池用正極では、電位負荷や副反応における酵素の劣化により無機化合物の触媒より使用耐久性が低いことがある。
<Catalyst for positive electrode of enzyme battery>
When an inorganic compound is used as a catalyst in the positive electrode of an enzyme battery, examples of oxygen reduction catalysts include noble metal catalysts, base metal oxide catalysts, carbon catalysts for enzyme batteries, and the like. A carbon catalyst is preferable from the viewpoint of cost.
A noble metal catalyst is a catalyst containing at least one element selected from ruthenium, rhodium, palladium, silver, osmium, iridium, platinum and gold among transition metal elements. These noble metal catalysts may be used alone or supported by other elements or compounds.
The base metal oxide catalyst contains at least one base metal element selected from the group consisting of zirconium, tantalum, titanium, niobium, vanadium, iron, manganese, cobalt, nickel, copper, zinc, chromium, tungsten, and molybdenum. Carbonitrides of these base metal elements and carbonitride oxides of these transition metal elements can be used more preferably.
A carbon catalyst for an enzyme cell (hereinafter also simply referred to as a carbon catalyst) is composed of a carbon material having a carbon element as a basic skeleton, and has physical and chemical interactions (bonds) between its constituent units, It is a catalyst material that contains heteroatoms such as heteroatoms such as N, B, and P, and optionally contains base metal elements, and has oxygen reduction activity. The base metal element referred to here is a metal element excluding noble metal elements (ruthenium, rhodium, palladium, silver, osmium, iridium, platinum, gold) among transition metal elements. Examples of base metal elements include cobalt, iron, nickel, It preferably contains one or more selected from the group consisting of manganese, copper, titanium, vanadium, chromium, zinc, and tin.
Containing a hetero element and a base metal element is significant in terms of oxygen reduction activity. Carbon catalysts for enzyme batteries have catalytic active sites such as nitrogen atoms introduced into the edges of the hexagonal mesh plane of carbon constituting the basic skeleton of the carbon material, carbon atoms in the vicinity thereof, and base metals on the surface of the catalyst. Nitrogen atoms and base metal atoms in a base metal-N4 structure in which four nitrogen atoms are aligned on a plane centering on an element can be mentioned.
Carbon catalysts for enzyme cells are conventionally known carbon catalysts prepared by mixing one or more carbon materials with a compound containing a nitrogen element and/or the base metal element and subjecting the mixture to heat treatment. can be used. The carbon material used for the carbon catalyst is not particularly limited as long as it is inorganic material-derived carbon particles and/or carbon particles obtained by heat-treating an organic material.
When an enzyme is used as a catalyst, any enzyme that can consume electrons can be used at the positive electrode of the enzyme battery. Enzymes can be used. A positive electrode for an enzyme battery using an oxygen reductase may have lower use durability than an inorganic compound catalyst due to potential load or deterioration of the enzyme due to side reactions.
＜セパレータ＞
セパレータとしては、負極と正極を電気的に分離できる（短絡の防止）ものであれば、特に限定されず従来公知の材料を用いる事ができる。具体的には、ポリエチレン繊維、ポリプロピレン繊維、ガラス繊維、樹脂不織布、ガラス不織布、フェルト、濾紙、和紙等を用いることができる。また、正極と負極が十分な距離を保ち接触による短絡が無い構造を取るならば、セパレータを用いなくてもよい。
<Separator>
The separator is not particularly limited as long as it can electrically separate the negative electrode and the positive electrode (prevention of short circuit), and conventionally known materials can be used. Specifically, polyethylene fiber, polypropylene fiber, glass fiber, resin nonwoven fabric, glass nonwoven fabric, felt, filter paper, Japanese paper, and the like can be used. Further, if a sufficient distance is maintained between the positive electrode and the negative electrode so that no short circuit occurs due to contact, the separator may not be used.
＜イオン伝導体＞
本発明におけるイオン伝導体はアノードとカソードの間でイオンの伝導を行うものである。イオン伝導体の形態はイオン伝導性を有するものであれば特に限定されるものではない。イオン伝導体としては、リン酸塩やナトリウム塩など電解質が溶けている電解液や、固体のポリマー電解質などを使用しても良い。
電解質はおむつに予め内蔵して利用しても良いし、尿中に含まれる電解質を利用して、その両方でも良い。
<Ionic conductor>
The ionic conductor in the present invention conducts ions between the anode and the cathode. The form of the ionic conductor is not particularly limited as long as it has ionic conductivity. As the ionic conductor, an electrolytic solution in which an electrolyte such as a phosphate or sodium salt is dissolved, or a solid polymer electrolyte may be used.
Electrolytes may be incorporated in diapers in advance and used, or electrolytes contained in urine may be used, and both may be used.
＜燃料＞
本願の酵素電池を動作させるために必要な燃料としては、酵素で分解できる有機物であれば特に限定はされず、Ｄ－グルコース等の単糖類、デンプン等の多糖類、有機酸などの有機物であれば幅広く利用できる。
おむつに搭載された酵素電池を動作させる場合では、燃料となる一種以上の有機物を予め酵素電池若しくはおむつに内蔵し、尿の水分中に有機物が溶出、拡散することで酵素電池を動作させたり、尿中に含まれる一種以上の有機物、例えばグルコースなどを利用して酵素電池を動作させたり、燃料となる一種以上の有機物を予め酵素電池若しくはおむつに内蔵し、尿の水分中に溶出した前記有機物と、尿中に含まれる一種以上の有機物を利用して、酵素電池を動作させたりできる。
予め燃料を内蔵する場合では、糖等の固体の燃料が好ましい。またコストや汎用性の観
点からグルコースを利用することが好ましい
<Fuel>
The fuel necessary for operating the enzyme cell of the present application is not particularly limited as long as it is an organic substance that can be decomposed by enzymes, and may be monosaccharides such as D-glucose, polysaccharides such as starch, or organic substances such as organic acids. widely available.
In the case of operating an enzyme battery mounted on a diaper, one or more kinds of organic substances that serve as fuel are incorporated in the enzyme battery or the diaper in advance, and the organic substance is eluted and diffused into the moisture of urine to operate the enzyme battery. One or more organic substances contained in urine, such as glucose, are used to operate an enzyme battery, or one or more organic substances that serve as fuel are incorporated in an enzyme battery or a diaper in advance, and the organic substance eluted into urine water. Then, one or more organic substances contained in the urine can be used to operate an enzyme battery.
When the fuel is incorporated in advance, a solid fuel such as sugar is preferable. In addition, it is preferable to use glucose from the viewpoint of cost and versatility.
本発明における酵素電池を搭載したおむつでは前述の様に、尿の供給により酵素電池で発電した電力を用いた電源やセンサー（水分、有機物）として機能できる。使い方としては、従来の抵抗検知型などのセンサー用の電源として本発明の酵素電池を利用したり、電源及びセンサーとして本発明の酵素電池を１種類以上利用したりすることができる。 As described above, the diaper equipped with the enzyme battery according to the present invention can function as a power supply and a sensor (moisture, organic matter) using the power generated by the enzyme battery by supplying urine. As for usage, the enzyme battery of the present invention can be used as a power source for sensors such as conventional resistance detection type sensors, or one or more types of the enzyme battery of the present invention can be used as power sources and sensors.
＜外部伝達手段を備えるシステム＞
本発明における酵素電池を搭載したおむつでは、無線送信機と組み合わせ、センシング情報をワイヤレスで外部に送信するシステムとして使うことができる。
例えば、排尿センサーの場合、予め燃料を内蔵し尿中の水分をセンシング対象とし、また同時に水分を利用し発電し得られた電力で無線送信機を作動したり、予め燃料を内蔵し尿中の水分を利用し発電し得られた電力で無線送信機及び別方式の排尿センサーを作動したり、また、尿糖値センサーの場合、尿中の糖を燃料及びセンシング対象として利用し、得られた電力で無線送信機を作動したり、尿中の糖をセンシング対象として利用し、予め燃料を内蔵し尿中の水分を利用し発電し得られた電力で無線送信機を作動したりできる。＜排尿量を演算する手段、有機物の濃度を演算する手段、排尿回数を演算する手段を備えるシステム＞
本発明における酵素電池を搭載したおむつでは、発電量、発電量変化は、排尿量、尿中の有機物の濃度、排尿回数などと相関することから、これらの情報から、排尿量、尿中の有機物の濃度、排尿回数を演算により求めるシステムとして使うことができる。演算された情報は、前記、外部伝達手段により、外部に送信することができる。
<System Equipped with External Transmission Means>
A diaper equipped with an enzyme battery according to the present invention can be combined with a wireless transmitter and used as a system for wirelessly transmitting sensing information to the outside.
For example, in the case of a urination sensor, fuel is contained in advance to detect water in urine, and at the same time, the water is used to generate electricity to operate a wireless transmitter. The power generated by using it can be used to operate a wireless transmitter and another type of urination sensor. It is possible to operate a wireless transmitter, use sugar in urine as a sensing target, and use the moisture in urine to generate electricity by incorporating fuel in advance and operate the wireless transmitter with the power obtained. <System Equipped with Means for Calculating Urination Amount, Means for Calculating Concentration of Organic Matter, and Means for Calculating Number of Urinations>
In the diaper equipped with the enzyme battery of the present invention, the amount of electricity generated and the change in the amount of electricity generated are correlated with the amount of urine output, the concentration of organic matter in urine, the number of times of urination, and the like. It can be used as a system for obtaining the concentration of and the number of times of urination by calculation. The calculated information can be transmitted to the outside by the external transmission means.
以下に、実施例により本発明をさらに具体的に説明するが、以下の実施例は本発明の権利範囲を何ら制限するものではない。なお、実施例および比較例における「部」は「質量部」、％は質量％を表す。 EXAMPLES The present invention will be described in more detail with reference to examples below, but the examples below do not limit the scope of the present invention. In the examples and comparative examples, "part" means "mass part" and % means % by mass.
＜酵素電池回路配線用導電炭素組成物の作製＞
鱗状黒鉛ＣＢ－１５０（日本黒鉛社製）を１８部、ファーネスブラックＶＵＬＣＡＮ（登録商標）ＸＣ７２（ＣＡＢＯＴ社製）を４．５部、バインダーとしてエマルション型アクリル樹脂分散溶液（トーヨーケム社製：Ｗ-１６８）を３部（固形分５０％）、分散剤
としてカルボキシメチルセルロース水溶液５０部（固形分２％）、溶剤として水４９．５部をミキサーに入れて混合し、更にサンドミルに入れて分散を行い、酵素電池回路配線用導電炭素組成物（１）を得た。
<Preparation of conductive carbon composition for enzyme battery circuit wiring>
18 parts of flaky graphite CB-150 (manufactured by Nippon Graphite Co., Ltd.), 4.5 parts of furnace black VULCAN (registered trademark) XC72 (manufactured by CABOT Co., Ltd.), emulsion type acrylic resin dispersion solution (manufactured by Toyochem Co., Ltd.: W-168) as a binder ) (solid content: 50%), 50 parts of carboxymethyl cellulose aqueous solution as a dispersant (solid content: 2%), and 49.5 parts of water as a solvent are mixed in a mixer, and then placed in a sand mill for dispersion. A conductive carbon composition (1) for circuit wiring of an enzyme battery was obtained.
＜酵素電池用回路配線の作製＞
前記酵素電池回路配線用導電炭素組成物（１）を、基材となる定性ろ紙Ｎｏ．１（アドバンテック社製）上にドクターブレードを用いて塗布した後、加熱乾燥し、導電層の厚さが８０μｍとなるよう調整し、酵素電池用回路配線（１）を得た。
<Preparation of circuit wiring for enzyme battery>
The conductive carbon composition (1) for circuit wiring of an enzyme battery was passed through a qualitative filter paper No. 1 serving as a base material. 1 (manufactured by Advantec Co., Ltd.), followed by heating and drying to adjust the thickness of the conductive layer to 80 μm, thereby obtaining Enzyme Battery Circuit Wiring (1).
＜酵素電池用導電性支持体の作製＞
酵素電池用回路配線と同様に、前記酵素電池回路配線用導電炭素組成物を、基材となる定性ろ紙Ｎｏ．１（アドバンテック社製）上にドクターブレードを用いて塗布した後、加熱乾燥し、導電層の厚さが８０μｍとなるよう調整した。長さ９ｃｍ幅８ｃｍの長方形に切り出したものを酵素電池用導電性支持体（１）とした。
<Preparation of conductive support for enzyme battery>
Similar to the circuit wiring for an enzyme battery, the conductive carbon composition for the circuit wiring for an enzyme battery was applied to a qualitative filter paper No. 2 serving as a base material. 1 (manufactured by Advantech) using a doctor blade and then dried by heating to adjust the thickness of the conductive layer to 80 μm. A rectangle with a length of 9 cm and a width of 8 cm was cut out and used as a conductive support for an enzyme battery (1).
＜酵素電池用負極の作製＞
導電性炭素材料としてファーネスブラックＶＵＬＣＡＮ（登録商標）ＸＣ７２（ＣＡＢＯＴ社製）の組成物をドクターブレードにより、導電性支持体（１）の片端に、加熱乾燥
後の導電性炭素材料の目付け量が２ｍｇ/ｃｍ２となるように塗布した後、メディエータ
としてテトラチアフルバレンのメタノール溶液と、負極触媒としてグルコースオキシダーゼ水溶液をそれぞれ滴下し、自然乾燥させ酵素電池用負極（１）を得た。
<Preparation of negative electrode for enzyme battery>
As a conductive carbon material, a composition of furnace black VULCAN (registered trademark) XC72 (manufactured by CABOT) was applied to one end of the conductive support (1) with a doctor blade so that the basis weight of the conductive carbon material after heat drying was 2 mg. /cm 2 , a methanol solution of tetrathiafulvalene as a mediator and an aqueous solution of glucose oxidase as a negative electrode catalyst were added dropwise, and dried naturally to obtain a negative electrode (1) for an enzyme battery.
＜酵素電池用炭素触媒の製造＞
［製造例１］
グラフェンナノプレートレットｘＧｎＰ－Ｃ－７５０（ＸＧｓｃｉｅｎｃｅ社製）と鉄フタロシアニン Ｐ－２６（山陽色素社製）を、質量比１／０．５（グラフェンナノプレ
ートレット／鉄フタロシアニン）となるようにそれぞれ秤量し、乾式混合を行い、混合物を
得た。上記混合物を、アルミナ製るつぼに充填し、電気炉にて窒素雰囲気下、８００℃で２時間熱処理を行い、酵素電池用炭素触媒（１）を得た。
<Production of carbon catalyst for enzyme battery>
[Production Example 1]
Graphene nanoplatelets xGnP-C-750 (manufactured by XGscience) and iron phthalocyanine P-26 (manufactured by Sanyo Color Co., Ltd.) were weighed so that the mass ratio was 1/0.5 (graphene nanoplatelets/iron phthalocyanine). and dry-blended to obtain a mixture. The mixture was filled in an alumina crucible and heat-treated at 800° C. for 2 hours in an electric furnace in a nitrogen atmosphere to obtain a carbon catalyst (1) for an enzyme cell.
＜酵素電池用正極の作製＞
酵素電池用炭素触媒（１）４．８部、水性液状媒体として水４９．２部、更に分散剤としてカルボキシメチルセルロース水溶液４０部（固形分２％）をミキサーに入れて混合し、更にサンドミルに入れて分散した。その後、バインダーとしてエマルション型アクリル樹脂分散溶液（トーヨーケム社製：Ｗ－１６８）６部（固形分５０％）を加えミキサーで混合し、酵素電池正極用電極組成物（１）を得た。
その後、酵素電池正極用電極組成物（１）を、ドクターブレードにより、導電性支持体（１）およびの片端に、乾燥後の酵素電池用炭素触媒の目付け量が２ｍｇ/ｃｍ２となる
ように塗布し、待機雰囲気中９５℃、６０分間乾燥し、酵素電池用正極（１）を得た。
<Preparation of positive electrode for enzyme battery>
4.8 parts of the carbon catalyst (1) for enzyme cells, 49.2 parts of water as an aqueous liquid medium, and 40 parts of an aqueous carboxymethylcellulose solution (2% solid content) as a dispersant were mixed in a mixer, and then placed in a sand mill. dispersed. After that, 6 parts of an emulsion-type acrylic resin dispersion solution (manufactured by Toyochem Co., Ltd.: W-168) (solid content: 50%) was added as a binder and mixed with a mixer to obtain an enzyme battery positive electrode composition (1).
After that, the enzyme battery positive electrode composition (1) was applied to one end of the conductive support (1) with a doctor blade so that the basis weight of the enzyme battery carbon catalyst after drying was 2 mg/cm 2 . It was applied and dried in a standby atmosphere at 95° C. for 60 minutes to obtain a positive electrode (1) for an enzyme battery.
＜酵素電池の作製＞
上記作製した酵素電池用回路配線、同正極、同負極に加えて、セパレータに燃料としてグルコース、イオン伝導体として塩化ナトリウムが担持された、ろ紙を貼り合わせて、酵素電池（１）を作製した。セパレータにグルコースと塩化ナトリウムを担持していない以外は同様の方法で、酵素電池（２）を作製した。
<Production of enzyme battery>
In addition to the circuit wiring for the enzyme battery, the positive electrode, and the negative electrode prepared above, filter paper carrying glucose as a fuel and sodium chloride as an ion conductor on the separator was pasted together to prepare an enzyme battery (1). An enzyme battery (2) was produced in the same manner, except that glucose and sodium chloride were not supported on the separator.
［実施例１～６］[比較例１]
＜酵素電池が搭載されたおむつの作製＞
トップシート、吸水材、およびバックシートからなる介護用おむつ（ライフリー４回分吸収用ユニ・チャーム社製）を解体し、おむつ内部の図１～３に示す位置に、上記で作製した酵素電池（１）をそれぞれに設置した後、元に戻し酵素電池が搭載されたおむつ（１）～（３）を作製した（実施例１～３）
また、酵素電池（１）を酵素電池（２）に変更した以外は酵素電池が搭載されたおむつ（１）～（３）と同様の方法で、酵素電池が搭載されたおむつ（４）～（６）を作製した（実施例４～６）。
また、酵素電池（１）を介護用おむつ（ライフリー４回分吸収用ユニ・チャーム社製）のトップシートの外側に両面テープで貼りつけ、酵素電池が搭載されておむつ（７）を作製した。（比較例１）
[Examples 1 to 6] [Comparative Example 1]
<Production of diaper equipped with enzyme battery>
A nursing care diaper (manufactured by Unicharm Co., Ltd. for absorbing 4 doses of Lifree) consisting of a top sheet, a water absorbing material, and a back sheet was disassembled, and the enzyme battery (1) prepared above was placed inside the diaper at the position shown in FIGS. ) respectively, and then returned to the original state to produce diapers (1) to (3) equipped with an enzyme battery (Examples 1 to 3)
In addition, diapers (4) to (4) equipped with an enzyme battery were prepared in the same manner as the diapers (1) to (3) equipped with an enzyme battery, except that the enzyme battery (1) was changed to the enzyme battery (2). 6) was produced (Examples 4 to 6).
Also, the enzyme battery (1) was attached to the outside of the top sheet of a nursing care diaper (manufactured by Unicharm Co., Ltd. for absorbing 4 doses of Lifree) with a double-faced tape to prepare a diaper (7) with the enzyme battery mounted thereon. (Comparative example 1)
＜無線通信回路の構築＞
上記作製した酵素電池について、昇圧コンバーター（ＬＴＣ３１０８ ストロベリーリ
ナックス（登録商標）社製）、無線モジュール（送信モジュール ＩＭ３１５ＴＸ、受信
モジュール ＩＭ３１５ＲＸ インタープラン社製）を、おむつ内の酵素電池から昇圧コ
ンバーターへ接続し、昇圧コンバーターから送信モジュールに接続、更に送信モジュールから発信された無線信号を受信モジュールで受信する無線通信回路を構築した。酵素電池正極（１）および負極（１）から昇圧コンバーターへの接続は、回路配線（１）を貼り合わせて行った。
<Construction of wireless communication circuit>
For the enzyme battery prepared above, a boost converter (LTC3108 manufactured by Strawberry Linux (registered trademark)) and a wireless module (transmitting module IM315TX, receiving module IM315RX manufactured by Interplan) are connected from the enzyme battery in the diaper to the boost converter, A wireless communication circuit was constructed in which the boost converter is connected to the transmission module, and the wireless signal transmitted from the transmission module is received by the reception module. The positive electrode (1) and negative electrode (1) of the enzyme battery were connected to the boost converter by bonding the circuit wiring (1).
＜酵素電池が搭載されたおむつの無線送信の評価＞
実施例１～３のおむつのトップシートに、尿中の水分を模擬し、超純水を投入したところ、いずれにおいても受信モジュールで信号の受信が確認された。これは、水の投入によって酵素電池まで到達した水中に、ろ紙内のグルコース及び塩化ナトリウムが溶解、拡散し、それぞれ燃料およびイオン伝導体として機能し酵素電池が発電していることを示している。実施例１および２のおむつであれば１５０ｍＬの水を一度に投入したところ無線の信号の受信が確認された。一方、実施例３のおむつの場合は６００ｍＬ以上の投入したところではじめて無線の信号の受信が確認された。これは、実施例３の場合では、吸水材の許容量を超えた段階ではじめて投入した水が酵素電池に到達し、発電が生じたためと考えられる。
実施例４～６に関して、超純水をグルコースが０．０１Ｍ溶解したｐＨ７の０．１Ｍリン酸緩衝液に変更した以外は、実施例１～３と同様の方法で、無線モジュールの動作を検証したところ、同様の挙動が見られた。これは尿中のグルコースを燃料として、機能し酵素電池が発電していることを示している。
<Evaluation of wireless transmission of diapers equipped with enzyme batteries>
When ultrapure water was added to the top sheets of the diapers of Examples 1 to 3 to simulate moisture in urine, signal reception by the receiving module was confirmed in all cases. This indicates that the glucose and sodium chloride in the filter paper are dissolved and diffused into the water that reaches the enzymatic battery by the injection of water, and function as a fuel and an ion conductor, respectively, and the enzymatic battery generates electricity. In the case of the diapers of Examples 1 and 2, when 150 mL of water was added at once, reception of wireless signals was confirmed. On the other hand, in the case of the diaper of Example 3, the reception of the wireless signal was confirmed only when 600 mL or more of the diaper was inserted. This is probably because, in the case of Example 3, the supplied water reached the enzyme cell for the first time when the allowable amount of the water absorbing material was exceeded, and power generation occurred.
Regarding Examples 4 to 6, the operation of the wireless module was verified in the same manner as in Examples 1 to 3, except that the ultrapure water was changed to 0.1 M phosphate buffer with pH 7 in which 0.01 M glucose was dissolved. Similar behavior was observed. This indicates that the enzyme battery functions and generates electricity using the glucose in the urine as fuel.
実施例１～６より、尿中の成分（水分や有機物）でおむつ内に搭載された酵素電池が駆動可能であることが明らかとなった。また同時に、電源不要で且つ、廃棄も容易で生体に安全な材料で構成された排尿センサーを搭載されたおむつが実現でき、また、発電した電力で送信機が動作することで、センシング情報をワイヤレス、例えば、受信機や携帯端末などに送信できることが可能になる。 From Examples 1 to 6, it became clear that the components (moisture and organic substances) in the urine can drive the enzyme battery mounted in the diaper. At the same time, it is possible to realize a diaper equipped with a urination sensor that does not require a power source, is easy to dispose of, and is made of materials that are safe for the body. , for example, can be transmitted to a receiver, a mobile terminal, or the like.
＜酵素電池が搭載されたおむつの安定駆動の評価＞
実施例４～６及び比較例１の酵素電池が搭載されたおむつを用いて、酵素電池の安定駆動の評価を行った。模擬尿としてグルコースが０．０１Ｍ溶解したｐＨ７の０．１Ｍリン酸緩衝液を用いた。実施例４～６及び比較例１のおむつを各４個ずつ作製し（ｌｏｔ１～４）、おむつの内側に模擬尿を投入し無線モジュールが動作するかを検証した。結果を表１に示す。
<Evaluation of stable driving of diaper equipped with enzyme battery>
Using the diapers in which the enzyme batteries of Examples 4 to 6 and Comparative Example 1 were mounted, stable operation of the enzyme batteries was evaluated. A pH 7 0.1 M phosphate buffer in which 0.01 M glucose was dissolved was used as simulated urine. Four diapers each of Examples 4 to 6 and Comparative Example 1 were produced (
安定駆動の評価基準を以下に示す。 Evaluation criteria for stable driving are shown below.
（安定駆動評価）
〇：無線モジュールが動作する
×：無線モジュールが動作しない
(Stable drive evaluation)
〇: Wireless module works ×: Wireless module does not work
表１より、実施例４～６のおむつは比較例１に比べ、酵素電池が安定して駆動できることがわかる。これは発電に必要な酵素電池内部への模擬尿の浸透において、酵素電池がトップシートの外側に露出している比較例１とは異なり、実施例４～６では、トップシートの内側にあることで親水的材料からなるトップシートや吸水材から酵素電池へ尿が十分に拡散、浸透されるため、安定した駆動に繋がったと考えられる。
From Table 1, it can be seen that the diapers of Examples 4 to 6 can stably drive the enzyme battery compared to Comparative Example 1. This is because, unlike Comparative Example 1, in which the enzyme battery is exposed outside the top sheet, the simulated urine penetrates inside the enzyme battery required for power generation, and in Examples 4 to 6, it is inside the top sheet. It is considered that the stable driving was achieved because the urine was sufficiently diffused and permeated from the top sheet and water-absorbing material made of a hydrophilic material into the enzyme cell.
［実施例７］
＜尿糖に対するセンシング能評価＞
酵素電池が搭載されたおむつ（４）の酵素電池用正極を作用極、酵素電池用負極を対極として、ポテンショ・ガルバノスタット（ＶｅｒｓａＳＴＡＴ３、Ｐｒｉｎｃｅｔｏｎ Ａｐｐｌｉｅｄ Ｒｅｓｅａｒｃｈ社製）に接続し、糖尿病患者の尿を模擬し、グルコース濃度が０.００１～０．０１Ｍ溶解したｐＨ７の０．１Ｍリン酸緩衝液を、おむつの内
側に投入し、室温下におけるＬＳＶ測定において、グルコース（センシング対象物）濃度に対する発電量の変化を調べた。その結果を図４に示す。
図４から明らかなように、グルコース濃度の変化に応じて比例的に発電量が変化することが見出されたことから、本発明により作製された酵素電池が搭載されたおむつ（４）では、発電量の履歴を調べることで尿中のグルコース濃度を検知できるセンサーとして使用できることが分かった。
[Example 7]
<Evaluation of sensing ability for urine sugar>
The positive electrode for the enzyme battery of the diaper (4) equipped with the enzyme battery was used as the working electrode, and the negative electrode for the enzyme battery was used as the counter electrode. Then, a 0.1M phosphate buffer solution with a pH of 7 in which 0.001 to 0.01M of glucose was dissolved was put inside the diaper, and in the LSV measurement at room temperature, the amount of power generation with respect to the glucose (sensing object) concentration was measured. examined the changes. The results are shown in FIG.
As is clear from FIG. 4, it was found that the power generation amount changed proportionally according to the change in glucose concentration. By examining the history of the amount of power generation, it was found that it can be used as a sensor that can detect the glucose concentration in urine.
［実施例８］
＜排尿量センシング＞
酵素電池が搭載されたおむつ（１）に１５０、３００、６００ｍＬの超純水をそれぞれ投入してから３０分経過後、酵素電池用正極を作用極、酵素電池用負極を対極として、ポテンショ・ガルバノスタット（ＶｅｒｓａＳＴＡＴ３、Ｐｒｉｎｃｅｔｏｎ Ａｐｐｌｉｅｄ Ｒｅｓｅａｒｃｈ社製）に接続し、室温下におけるＬＳＶ測定から発電量を調べた。その結果を図５に示す。
図５から明らかなように、超純水の投入量に応じて比例的に発電量が減衰することが見出された。これは投入した液量に応じて、燃料として内蔵したグルコースが溶出し、残存したグルコース量に応じた発電量となっていることを示している。このことから酵素電池が搭載されたおむつ（１）では、残存している燃料の量に応じた発電量を調べることで、排尿量をセンシング出来る可能性が示唆された。
[Example 8]
<Urination amount sensing>
30 minutes after 150, 300, and 600 mL of ultrapure water were added to the diaper (1) equipped with the enzyme battery, the positive electrode for the enzyme battery was used as the working electrode, and the negative electrode for the enzyme battery was used as the counter electrode. It was connected to a stat (VersaSTAT3, manufactured by Princeton Applied Research), and the power generation amount was examined by LSV measurement at room temperature. The results are shown in FIG.
As is clear from FIG. 5, it was found that the amount of power generation attenuated proportionally according to the amount of ultrapure water input. This indicates that the glucose contained as fuel is eluted according to the amount of liquid introduced, and that the amount of power generation corresponds to the amount of residual glucose. From this, it was suggested that the diaper (1) equipped with the enzyme battery may be able to sense the amount of urination by examining the amount of power generated according to the amount of remaining fuel.
［実施例９］
＜排尿回数センシング＞
実施例４の酵素電池が搭載されたおむつを用いて１５０ｍＬの擬似尿として超純水を投入後、９０分及び１８０分経過後に、更にそれぞれ１５０ｍＬの超純水を投入し、無線モジュールが動作するかを検証した。その結果を表２に示す。
表２から明らかなように、超純水の投入直後においてのみ無線モジュールの動作が確認された。
これは超純水投入後９０分経過した状態に比べ超純水投入直後では、酵素電池内部が十分に濡れており、反応に必要なイオンの拡散が十分に生じ、送信モジュールの動作に必要な発電量を得る事ができたためと考えられる。これにより、液の投入による発電量の変化を検出し、排尿回数をセンシング可能であることが分かった。
[Example 9]
<Urination frequency sensing>
After 150 mL of ultrapure water was added as simulated urine using the diaper equipped with the enzyme battery of Example 4, 150 mL of ultrapure water was further added after 90 minutes and 180 minutes, and the wireless module operated. verified whether Table 2 shows the results.
As is clear from Table 2, the operation of the wireless module was confirmed only immediately after the ultrapure water was added.
This is because the inside of the enzyme cell is sufficiently wet immediately after the addition of ultrapure water, compared to the
（無線の動作）
〇：無線モジュールが動作する
×：無線モジュールが動作しない
(radio operation)
〇: Wireless module works ×: Wireless module does not work
１・・・酵素電池、２・・・トップシート、３・・・吸水材、４・・・バックシート
DESCRIPTION OF
Claims (11)
前記酵素電池は、正極および、負極を含んでなり、
前記正極または前記負極の少なくとも一方が酵素を含むことを特徴とする酵素電池が搭載されたおむつ。 A diaper comprising at least a topsheet, a water-absorbent material, and a backsheet as constituent members, wherein an enzyme battery is positioned between the topsheet and the backsheet,
The enzyme battery comprises a positive electrode and a negative electrode,
A diaper equipped with an enzyme battery, wherein at least one of the positive electrode and the negative electrode contains an enzyme.
記載のおむつ。 The diaper according to any one of claims 1 to 6, which contains an enzyme capable of generating electricity from one or more kinds of organic matter contained in urine.
機物の濃度を演算する手段を備えるシステム。 8. A system using the diaper according to claim 7, comprising means for calculating the concentration of one or more organic substances contained in urine from the amount of power generated by the enzyme battery.
11. The system according to any one of claims 8 to 10, further comprising an external transmission means interlocked with the power generation of the enzyme battery.
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| JP2011165464A (en) * | 2010-02-09 | 2011-08-25 | Mitsubishi Rayon Co Ltd | Fuel cell |
| JP2013094175A (en) * | 2011-10-27 | 2013-05-20 | Unicharm Corp | Electromotive module and disposable wearing article |
| JP2013157317A (en) * | 2012-01-05 | 2013-08-15 | Toyo Ink Sc Holdings Co Ltd | Catalyst paste composition for fuel cell, catalyst layer formed using the same, and joined body |
| WO2018062419A1 (en) * | 2016-09-30 | 2018-04-05 | 学校法人東京理科大学 | Power generation device, power generation method, and concentration measurement method |
| JP2018068583A (en) * | 2016-10-28 | 2018-05-10 | 学校法人立命館 | Urine detection electrode, manufacturing method thereof, and urine detection device |
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| JP2011165464A (en) * | 2010-02-09 | 2011-08-25 | Mitsubishi Rayon Co Ltd | Fuel cell |
| JP2013094175A (en) * | 2011-10-27 | 2013-05-20 | Unicharm Corp | Electromotive module and disposable wearing article |
| JP2013157317A (en) * | 2012-01-05 | 2013-08-15 | Toyo Ink Sc Holdings Co Ltd | Catalyst paste composition for fuel cell, catalyst layer formed using the same, and joined body |
| WO2018062419A1 (en) * | 2016-09-30 | 2018-04-05 | 学校法人東京理科大学 | Power generation device, power generation method, and concentration measurement method |
| JP2018068583A (en) * | 2016-10-28 | 2018-05-10 | 学校法人立命館 | Urine detection electrode, manufacturing method thereof, and urine detection device |
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