JP2001241599A - Hydrogen recovery and storage container - Google Patents
Hydrogen recovery and storage containerInfo
- Publication number
- JP2001241599A JP2001241599A JP2000049541A JP2000049541A JP2001241599A JP 2001241599 A JP2001241599 A JP 2001241599A JP 2000049541 A JP2000049541 A JP 2000049541A JP 2000049541 A JP2000049541 A JP 2000049541A JP 2001241599 A JP2001241599 A JP 2001241599A
- Authority
- JP
- Japan
- Prior art keywords
- hydrogen
- sheet
- storage
- gas
- container
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
Classifications
-
- 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
- Y02E60/32—Hydrogen storage
-
- 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
-
- 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
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/10—Internal combustion engine [ICE] based vehicles
- Y02T10/30—Use of alternative fuels, e.g. biofuels
Landscapes
- Filling Or Discharging Of Gas Storage Vessels (AREA)
- Hydrogen, Water And Hydrids (AREA)
- Fuel Cell (AREA)
Abstract
(57)【要約】
【課題】 天然ガスやメタノールを改質することによっ
て得られる水素と他の不純物ガスから構成される混合ガ
ス（改質ガス）等より、水を効率良く分離回収し、その
水素を貯蔵する機能を持つとともに、水素を供給する水
素タンクとしての機能をも併せ持つ水素回収貯蔵容器お
よび装置を提供すること。
【解決手段】 水素吸蔵合金に結着剤を加えてペースト
状とし、金属多孔質体シートに塗布又は充填した後、加
圧成形した水素吸蔵性シートを積層して、ガス入り口と
ガス出口とを備えた容器内に収納してなることを特徴と
する水素回収・貯蔵容器である。また、前記水素吸蔵性
シートに、さらに多孔体シートを重ねて張り合わせ積層
したものが好ましい。
PROBLEM TO BE SOLVED: To efficiently separate and recover water from a mixed gas (reformed gas) composed of hydrogen and other impurity gas obtained by reforming natural gas or methanol, and to obtain the water. To provide a hydrogen recovery storage container and a device having a function of storing hydrogen and also having a function as a hydrogen tank for supplying hydrogen. SOLUTION: A binder is added to a hydrogen storage alloy to form a paste, and after coating or filling a metal porous sheet, a pressure-formed hydrogen storage sheet is laminated to form a gas inlet and a gas outlet. A hydrogen recovery / storage container characterized by being housed in a container provided. Further, it is preferable that a porous sheet is further laminated on the hydrogen storage sheet and laminated.
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、水素運搬用、水素
エンジン用あるいは燃料電池などの分野で用いられる水
素回収・貯蔵容器に関する。さらに詳しくは、水素及び
水素を含む混合ガスからの水素回収、水素貯蔵、水素放
出用の装置に適用される水素回収・貯蔵容器に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a hydrogen recovery / storage container used in the fields of hydrogen transport, hydrogen engines, fuel cells, and the like. More specifically, the present invention relates to a hydrogen recovery / storage container applied to a device for recovering hydrogen from hydrogen and a mixed gas containing hydrogen, storing hydrogen, and releasing hydrogen.
【０００２】[0002]
【従来の技術】近年、石油の代替エネルギーとして、水
素を発電用燃料として使用する燃料電池が注目を集めて
いる。この燃料電池は、燃料極と酸化剤極からなり、燃
料極には水素を、そして酸化剤極には酸素を供給し、電
解質層を介して接触させ電気化学反応により発生する電
気エネルギーを両極から取り出すようにしたものであ
る。この種の燃料電池においては、燃料として水素が使
用されている。この水素は、一般に、天然ガス，ナフ
サ，液化石油ガス等の炭化水素（水素含有改質ガス）燃
料を改質し、水素を主成分とする燃料ガスに変換するこ
とにより得られることが知られている。2. Description of the Related Art In recent years, fuel cells using hydrogen as a fuel for power generation as an alternative energy to petroleum have attracted attention. This fuel cell is composed of a fuel electrode and an oxidant electrode.Hydrogen is supplied to the fuel electrode and oxygen is supplied to the oxidant electrode. It is intended to be taken out. In this type of fuel cell, hydrogen is used as fuel. It is known that this hydrogen is generally obtained by reforming a hydrocarbon (hydrogen-containing reformed gas) fuel such as natural gas, naphtha, liquefied petroleum gas, etc., and converting it to a fuel gas containing hydrogen as a main component. ing.
【０００３】この際必要とされる水素吸蔵合金を用いた
水素の貯蔵装置や微量の不純物ガスを含む水素の精製装
置は、従来より多くの提案がなされている。しかし、水
素含有量が５０〜７０％と低く、他の不純物ガスを多量
に含むメタノール改質ガス等のいわゆる混合ガスから、
水素を効率良く回収しそれを貯蔵する容器や装置は提案
されていない。それは、これまでの水素吸蔵合金を収納
した容器のガス導入口が一箇所であり、そこから混合ガ
スを容器内に導入し水素を吸蔵させた後、同じ導入口か
ら残ガスの排出と水素ガスの供給を行う方式のためであ
る。この方式では、混合ガスから水素を回収していくに
伴って不純物ガスの蓄積が起こり、その結果、水素の回
収効率が大きく減少する。また、水素の貯蔵媒体として
使用される水素吸蔵合金は、水素の吸蔵放出に伴って体
積変化を起こし微粉となっていくため、使用を繰り返す
と容器内で偏りを起こし、一定の性能を維持することが
困難であった。[0003] Many proposals have been made for a hydrogen storage device using a hydrogen storage alloy and a hydrogen purification device containing a trace amount of impurity gas, which are required at this time. However, from a so-called mixed gas such as a methanol reformed gas having a low hydrogen content of 50 to 70% and containing a large amount of another impurity gas,
No container or device for efficiently recovering and storing hydrogen has been proposed. This is because the gas inlet of the container that has stored the hydrogen storage alloy is a single point, a mixed gas is introduced into the container from there, and hydrogen is occluded. This is because of the method of supplying the water. In this method, impurity gas accumulates as hydrogen is recovered from the mixed gas, and as a result, hydrogen recovery efficiency is greatly reduced. In addition, since the hydrogen storage alloy used as a hydrogen storage medium changes its volume with the storage and release of hydrogen and becomes fine powder, repeated use causes a bias in the container and maintains a constant performance. It was difficult.
【０００４】[0004]
【発明が解決しようとする課題】このような状況下で、
本発明の目的は、天然ガスやメタノールを改質すること
によって得られる水素と他の不純物ガスから構成される
混合ガス（改質ガス）等より、水を効率良く分離回収
し、その水素を貯蔵する機能を持つとともに、水素を供
給する水素タンクとしての機能をも併せ持つ水素回収貯
蔵容器および装置を提供することである。In such a situation,
An object of the present invention is to efficiently separate and recover water from a mixed gas (reformed gas) composed of hydrogen and other impurity gases obtained by reforming natural gas or methanol and store the hydrogen. It is an object of the present invention to provide a hydrogen recovery storage container and an apparatus having a function of performing a hydrogen supply and a function as a hydrogen tank for supplying hydrogen.
【０００５】[0005]
【課題を解決するための手段】本発明者らは、上記目的
を達成するために鋭意研究した結果、これまで水素ガス
純度の低い混合ガスから、水素ガスだけが水素吸蔵合金
に吸収される過程を詳細に検討した結果、水素吸蔵合金
の表面上に混合ガスを連続して流す事によって、水素の
回収効率が飛躍的に向上することを見い出した。水素吸
蔵合金に結着剤を加えて加圧成形した特定の水素吸蔵性
シートを、ガス入り口とガス出口とを有する容器に収納
してガスフローをすることが有効であることを知見し、
本発明を完成するに至った。すなわち本発明は、（１）
水素吸蔵合金に結着剤を加えてペースト状とし、金属多
孔質体シートに塗布又は充填した後、加圧成形した水素
吸蔵性シートを積層して、ガス入り口とガス出口とを備
えた容器内に収納してなることを特徴とする水素回収・
貯蔵容器、（２）前記水素吸蔵性シートに、さらに多孔
体シートを重ねて張り合わせ積層したことからなる前記
（１）の水素回収・貯蔵容器、（３）前記水素吸蔵性シ
ートを、さらに多孔体シートと重ね合せて巻回したこと
を特徴とする前記（１）の水素回収・貯蔵容器、（４）
前記（３）により水素吸蔵性シートを巻回して得られた
筒状体を長手方向に分割した後、その分割体を複数個並
べて容器内に収納したことを特徴とする前記（１）の水
素回収・貯蔵容器、（５）水素回収・貯蔵容器の複数個
を、直列あるいは並列に配置したことを特徴とする前記
（１）〜（４）のいずれかの水素回収貯蔵装置、（６）
ガス入口とガス出口とを有し、かつガスヘッダーを備え
た密閉容器内に、水素吸蔵性シートを巻回して収納して
ある筒状内管が複数個並設されており、該筒状内管は上
下のガスヘッダーに連結していると共に、密閉容器内の
空隙部には熱媒体を流入するように形成されていること
を特徴とする前記（１）及び（３）〜（５）のいずれか
の水素回収・貯蔵容器、及び（７）ガス入口とガス出口
とを有した密閉容器内に、平板状からなる前記（１）の
水素吸蔵性シートを複数枚積層して収納されていると共
に、該シートと密閉容器側面とを貫通して熱媒体用の流
入管が複数本並設されていることを特徴とする前記
（１）、（２）及び（５）のいずれかの水素回収・貯蔵
容器、（８）前記水素回収・貯蔵容器は、燃料改質装置
の運転中に生成する改質ガス中に含まれる水素を選択的
に吸蔵し、また、吸蔵した水素を放出タンクに供給する
ために用いられることを特徴とする前記（１）〜（７）
のいずれかの燃料電池用水素回収・貯蔵容器を提供する
ものである。Means for Solving the Problems The inventors of the present invention have conducted intensive studies to achieve the above object, and as a result, a process in which only a hydrogen gas is absorbed by a hydrogen storage alloy from a mixed gas having a low hydrogen gas purity. As a result of a detailed study, it was found that by continuously flowing the mixed gas on the surface of the hydrogen storage alloy, the hydrogen recovery efficiency was dramatically improved. Finding that it is effective to carry out gas flow by storing a specific hydrogen storage sheet press-formed by adding a binder to the hydrogen storage alloy in a container having a gas inlet and a gas outlet,
The present invention has been completed. That is, the present invention provides (1)
After adding a binder to the hydrogen-absorbing alloy to form a paste and applying or filling the porous metal sheet, the pressure-molded hydrogen-absorbing sheet is laminated, and the container is provided with a gas inlet and a gas outlet. Hydrogen recovery characterized by being stored in
A storage container, (2) a hydrogen recovery / storage container according to (1), wherein a porous sheet is further laminated on the hydrogen storage sheet, and (3) the hydrogen storage sheet is further used as a porous body. (4) the hydrogen recovery / storage container according to (1), wherein the hydrogen recovery and storage container is wound while being superposed on a sheet.
The hydrogen according to (1), wherein the tubular body obtained by winding the hydrogen storage sheet according to (3) is divided in the longitudinal direction, and a plurality of the divided bodies are arranged and stored in a container. (5) A hydrogen recovery / storage device according to any one of (1) to (4), wherein a plurality of hydrogen recovery / storage containers are arranged in series or in parallel.
In an airtight container having a gas inlet and a gas outlet, and provided with a gas header, a plurality of tubular inner tubes in which a hydrogen-absorbing sheet is wound and housed are arranged side by side. (1) and (3) to (5), wherein the pipe is connected to the upper and lower gas headers and is formed so as to allow a heat medium to flow into a gap in the closed vessel. In one of the hydrogen recovery / storage containers and (7) an airtight container having a gas inlet and a gas outlet, a plurality of the flat hydrogen-absorbing sheets of the above (1) are stacked and stored. And a plurality of heat medium inflow pipes penetrating through the sheet and the side surface of the airtight container, and wherein a plurality of heat medium inflow pipes are provided side by side. (1), (2) and (5)・ Storage container, (8) The hydrogen recovery / storage container is provided with a reformer generated during the operation of the fuel reformer. Selectively absorbing hydrogen contained in the gas, also characterized in that it is used to supply the occluded hydrogen discharge tank (1) to (7)
The present invention also provides a hydrogen recovery / storage container for a fuel cell.
【０００６】[0006]
【発明の実施の形態】本発明で用いられる水素吸蔵性シ
ートは、水素吸蔵合金に結着剤（バインダー）を加えて
ペースト状にし、金属多孔質体シートに塗布又は充填し
た後、加圧成形して得られる。ここで、金属多孔質体と
は、連続気孔構造を有する金属発泡体、或いは金属の細
線からなる織布，不織布，金属製パンチプレート等など
の総称をいう。かかる金属多孔質体を構成する金属とし
ては、銅，アルミニウム，ニッケル，コバルト，亜鉛等
の熱伝導効率が高い金属が挙げられる。特に軽量化の観
点からは、アルミニウムが好ましい。また結着剤として
は、例えばポリテトラフルオロエチレンなどが挙げられ
る。この結着剤は、主として水素吸蔵合金粉末を固定す
るために用いるのであるが、水素吸蔵合金粉末表面の被
毒を抑制する効果をも有する。なお、本発明の水素回収
・貯蔵容器に用いられる水素吸蔵合金としては通常用い
られるものであればよく、例えばＬａＮｉ合金，ミッシ
ュメタル系合金，Ｔｉ−Ｚｒ−Ｍｎ−Ｃｒ−Ｃｕ合金な
どが挙げられる。BEST MODE FOR CARRYING OUT THE INVENTION The hydrogen-absorbing sheet used in the present invention is formed into a paste by adding a binder to a hydrogen-absorbing alloy, applied or filled to a porous metal sheet, and then press-formed. Is obtained. Here, the metal porous body is a general term for a metal foam having a continuous pore structure, a woven fabric, a nonwoven fabric, a metal punch plate, or the like made of a thin metal wire. Examples of the metal constituting such a porous metal body include metals having high heat conduction efficiency, such as copper, aluminum, nickel, cobalt, and zinc. Particularly, from the viewpoint of weight reduction, aluminum is preferable. Examples of the binder include polytetrafluoroethylene. This binder is mainly used for fixing the hydrogen storage alloy powder, but also has an effect of suppressing poisoning of the surface of the hydrogen storage alloy powder. The hydrogen storage alloy used for the hydrogen recovery / storage container of the present invention may be any commonly used hydrogen storage alloy, such as a LaNi alloy, a misch metal alloy, a Ti—Zr—Mn—Cr—Cu alloy. .
【０００７】本発明における前記水素吸蔵性シートは、
さらに多孔体シートを重ねて張り合わせ平板状などに積
層されたもの、或いはさらに多孔体シートと重ね合せて
巻回されたものが好ましい。ここで、多孔体シートと
は、前記の金属多孔質体の外にプラスチックス又は有機
質の多孔質体などが挙げられ含まれ、多孔体シートには
ペーストは含まれていない。このように、水素吸蔵性シ
ート（例えば図１における１）を多孔体シート（例えば
図１における１’）と重ねて二重シートとしたものを積
層した場合は、導入ガスが水素吸蔵合金粉末と、より均
一に接触することができるので、特に本発明におけるガ
スフロータイプにおいて混合ガスからの水素の効率的回
収が可能である。本発明の水素回収・貯蔵容器におい
て、上記の水素吸蔵性シート１は、例えば、図１に示す
ように、渦巻状に巻回されて円筒状積層シート２を形成
し、筒状内管３に収納され、該筒状内管の上下面に各々
水素含有ガスの導入口４と放出口４’とを設けることが
できる。ここで、水素回収・貯蔵容器の複数個を、直列
あるいは並列に配置してもよい。また、本発明で用いる
水素吸蔵性シートの形態の他の例として、図２に示す水
素吸蔵性シートは、平板状に成形されたシート５であ
り、この複数枚を積層して箱型密閉容器６に収納され、
この容器の両側面又は上下面の外側の任意の位置に水素
含有ガスの導入口７と放出口７’とを設けることができ
る。ここで、水素回収・貯蔵容器の複数個を、直列ある
いは並列に配置してもよい。In the present invention, the hydrogen storage sheet is
Further, a porous sheet is preferably laminated and laminated in a flat plate shape or the like, or a laminated sheet is further laminated and wound on a porous sheet. Here, the porous body sheet includes, in addition to the metal porous body, plastics or organic porous bodies, and the like, and the porous sheet does not include paste. As described above, when the hydrogen storage sheet (for example, 1 in FIG. 1) and the porous sheet (for example, 1 ′ in FIG. 1) are stacked to form a double sheet, the introduced gas is the same as the hydrogen storage alloy powder. , More efficiently, the hydrogen can be efficiently recovered from the mixed gas, particularly in the gas flow type of the present invention. In the hydrogen recovery / storage container of the present invention, the above-mentioned hydrogen storage sheet 1 is spirally wound to form a cylindrical laminated sheet 2 as shown in FIG. An inlet 4 and an outlet 4 ′ for the hydrogen-containing gas can be provided on the upper and lower surfaces of the tubular inner tube. Here, a plurality of hydrogen recovery / storage containers may be arranged in series or in parallel. As another example of the form of the hydrogen-absorbing sheet used in the present invention, the hydrogen-absorbing sheet shown in FIG. 2 is a sheet 5 formed into a flat plate shape. 6
An inlet 7 and an outlet 7 'for the hydrogen-containing gas can be provided at arbitrary positions outside both sides or upper and lower surfaces of the container. Here, a plurality of hydrogen recovery / storage containers may be arranged in series or in parallel.
【０００８】次に、特に燃料電池用として適用される本
発明の水素回収・貯蔵容器について、図３〜図７により
詳細に説明する。本発明において好適な水素回収・貯蔵
容器の第１の形態は、少なくとも一個のガス出入管を有
し、かつガスヘッダー１０を備えた密閉容器８の内部
に、前記の水素吸蔵シートを巻回して収納してある筒状
内管３が複数個並設されており、該筒状内管は上下のガ
スヘッダー１０に連結していると共に、密閉容器内の空
隙部には熱媒体が流入するように形成されている水素回
収・貯蔵容器である。ここで、密閉容器はガスの入口と
出口とを有するガスフロータイプのものである。また、
筒状内管の形状は特に限定されるものではないが、円筒
形容器の場合には、該円筒容器内のガス圧が高くても変
形し難い。従って容器の軽量化も可能である。なお、密
閉容器８については特に耐圧性を必要としない。Next, the hydrogen recovery / storage container of the present invention particularly applied to a fuel cell will be described in detail with reference to FIGS. A first embodiment of a hydrogen recovery / storage container suitable for the present invention is to wind the above-mentioned hydrogen storage sheet inside a closed container 8 having at least one gas inlet / outlet pipe and having a gas header 10. A plurality of stored tubular inner tubes 3 are juxtaposed, and the tubular inner tubes are connected to the upper and lower gas headers 10 so that the heat medium flows into the gap in the sealed container. This is a hydrogen recovery and storage container formed in. Here, the closed container is of a gas flow type having an inlet and an outlet for gas. Also,
The shape of the cylindrical inner tube is not particularly limited, but in the case of a cylindrical container, it is difficult to deform even if the gas pressure in the cylindrical container is high. Therefore, the weight of the container can be reduced. Note that the sealed container 8 does not particularly require pressure resistance.
【０００９】さらに図３により具体的に説明すれば、本
発明に係る水素回収・貯蔵容器は、方形の密閉容器８の
上下面に各々ガス導入管９と放出管９’とを有すると共
にガスヘッダー１０、１０’が配設されている。そし
て、密閉容器８には、水素吸蔵シートを渦巻状に巻回し
た状態で収納されている筒状内管３が並設されると共
に、該筒状内管３は密閉容器８の上下面で各々ガスヘッ
ダー１０、１０’とパイプ１１，１１’を介して連絡し
ている。そして、筒状内管３を加熱又は冷却するために
密閉容器８の側面外側には、熱媒用管１２，１２’が設
けられている。また、上記の第１の形態の他の例とし
て、図４に示す水素回収・貯蔵容器は、円柱形からなる
容器内に、水素吸蔵シートを渦巻状に巻回した状態で収
納されている筒状流通管が配設されており、その作用は
前記の場合と同様である。More specifically, referring to FIG. 3, the hydrogen recovery / storage container according to the present invention has a gas inlet tube 9 and a discharge tube 9 'on the upper and lower surfaces of a rectangular sealed container 8, respectively, and a gas header. 10, 10 'are provided. The sealed container 8 is provided with the tubular inner pipes 3 in which the hydrogen storage sheet is spirally wound and accommodated therein, and the tubular inner pipes 3 are arranged on the upper and lower surfaces of the sealed container 8. The gas headers 10 and 10 'are connected to each other via pipes 11 and 11'. Heat medium pipes 12 and 12 ′ are provided outside the side surface of the sealed container 8 for heating or cooling the cylindrical inner pipe 3. Further, as another example of the first embodiment, the hydrogen recovery / storage container shown in FIG. 4 is a cylinder in which a hydrogen storage sheet is spirally wound in a cylindrical container. A flow pipe is provided, the operation of which is the same as described above.
【００１０】また、本発明において好適な水素回収・貯
蔵容器の第２の形態は、少なくとも一個のガス出入管を
有した密閉容器１３の内部に、平板状からなる水素吸蔵
性シートが複数枚積層して収納されていると共に、該シ
ートの積層体１４と密閉容器１３の側面とを貫通して熱
媒体用の流入管１６が複数本並設されている水素回収・
貯蔵容器である。ここで、密閉容器はガス入口とガス出
口とを有するガスフロータイプのものである。また、こ
の構造で用いられる平板状の水素吸蔵性シートの積層状
態は、互いに接していてもよいが、各シート毎に所望の
間隔をもって並設されたものでもよい。これらの平板状
の水素吸蔵性シートはそれ自体の形状よりフィン構造を
兼ねることができる。さらに、図５により具体的に説明
すれば、本発明に係る水素回収・貯蔵容器は、密閉容器
１３の内部に平板状の水素吸蔵性シートが複数枚積層さ
れて収納してあると共に、密閉容器１３の上下面には、
各々ガス導入管１５と放出管１５’が設けられている。
そして、水素吸蔵性シート積層体１４と密閉容器１３の
側面とを貫通して、水素吸蔵性シートを加熱又は冷却す
るための熱媒管１６が配設されている。A second preferred embodiment of the hydrogen recovery / storage container according to the present invention is that a plurality of flat hydrogen storage sheets are laminated inside a closed container 13 having at least one gas inlet / outlet pipe. And a plurality of heat medium inflow pipes 16 penetrating through the sheet laminate 14 and the side surface of the sealed container 13.
It is a storage container. Here, the closed container is of a gas flow type having a gas inlet and a gas outlet. The lamination state of the flat hydrogen-absorbing sheets used in this structure may be in contact with each other, or may be arranged side by side at a desired interval for each sheet. These flat hydrogen-absorbing sheets can also have a fin structure rather than their own shape. More specifically, referring to FIG. 5, the hydrogen recovery / storage container according to the present invention includes a plurality of flat hydrogen-absorbing sheets stacked inside a closed container 13 and stored therein. 13 on the upper and lower surfaces,
Each is provided with a gas inlet pipe 15 and a discharge pipe 15 '.
Further, a heat medium pipe 16 for heating or cooling the hydrogen storage sheet is provided so as to penetrate the hydrogen storage sheet laminate 14 and the side surface of the closed container 13.
【００１１】本発明による前記の構成からなる水素回収
・貯蔵容器によれば、水素吸蔵合金の表面上に混合ガス
を連続して流すことによって、水素の回収効率が飛躍的
に向上する。すなわち、混合ガス中の水素が、水素吸蔵
合金中に吸収される始めると、合金表面の残ガス中の水
素濃度は減少していき、水素の分圧は小さくなる。水素
の分圧が、水素吸蔵合金の平衡圧より低くなれば水素の
吸蔵は停止する。一方、本発明では、水素吸蔵合金表面
上に連続して混合ガスを流すことにより、水素以外の不
純物ガスを出口より排出し、合金表面上の水素ガス濃度
を一定にする事によって水素を効率よく回収することが
できる。また、所定の粒度に粉砕された粉状の水素吸蔵
合金を、金属の薄体表面にバインダーを用いて塗布し、
その後圧延することで合金粉を保持し、それに接するよ
うに多孔体上のフィルムを配して、ガスの流路を形成す
ることによって、合金粉が容器内で偏在する事が防止さ
れる。さらに、ガス流路の効果によって混合ガスの導入
量を一定に制御することが可能である。また、水素吸蔵
合金へのガスの接触も常に一定であるため、回収／貯蔵
／放出のサイクルを繰り返しても回収効率が減少するこ
とはない。According to the hydrogen recovery / storage container having the above-mentioned structure according to the present invention, by continuously flowing the mixed gas on the surface of the hydrogen storage alloy, the efficiency of recovering hydrogen is greatly improved. That is, when the hydrogen in the mixed gas starts to be absorbed into the hydrogen storage alloy, the hydrogen concentration in the residual gas on the alloy surface decreases, and the partial pressure of hydrogen decreases. When the partial pressure of hydrogen becomes lower than the equilibrium pressure of the hydrogen storage alloy, the storage of hydrogen stops. On the other hand, in the present invention, by flowing a mixed gas continuously on the surface of the hydrogen storage alloy, impurity gas other than hydrogen is discharged from the outlet, and the hydrogen gas concentration on the surface of the alloy is kept constant to efficiently generate hydrogen. Can be recovered. Also, a powdery hydrogen storage alloy pulverized to a predetermined particle size is applied to a thin metal surface using a binder,
Thereafter, the alloy powder is held by rolling, and a film on a porous body is arranged so as to be in contact with the alloy powder, and a gas flow path is formed, thereby preventing uneven distribution of the alloy powder in the container. Further, the introduction amount of the mixed gas can be controlled to be constant by the effect of the gas flow path. Also, since the gas contact with the hydrogen storage alloy is always constant, the recovery efficiency does not decrease even if the recovery / storage / release cycle is repeated.
【００１２】さらに、前記水素吸蔵性シートと多孔体シ
ートとを重ねて張り合わせ又は巻回積層した場合には、
伝熱性の改良により水素の急速吸蔵・放出が可能であ
り、また不純物の通過が容易となるために水素の回収率
は向上し、さらに、ガス流れの制御が容易となる。ま
た、水素吸蔵性シートを巻回して得られた筒状体を長手
方向に分割した後、その分割体を不連続に複数個並べて
容器内に収納した場合には、流れの集中（パス）が防止
され、ガスはより均一に水素吸蔵合金と接触することが
できる。Further, when the hydrogen-absorbing sheet and the porous sheet are laminated and wound or laminated,
The improved heat transfer allows rapid absorption and desorption of hydrogen, facilitates the passage of impurities, improves the recovery of hydrogen, and facilitates the control of gas flow. In addition, when a tubular body obtained by winding a hydrogen storage sheet is divided in the longitudinal direction, and then a plurality of the divided bodies are arranged in a discontinuous manner and stored in a container, the flow concentration (path) is reduced. Is prevented and the gas can contact the hydrogen storage alloy more uniformly.
【００１３】本発明において、前記の水素回収・貯蔵容
器は、図６に示す如く、燃料電池システムの水素吸蔵タ
ンク２０として用いられる。ところで、一般的な水素供
給装置において、吸蔵タンク２０は、天然ガス，メタノ
ール，メッサ，石炭等の燃料ガスを、燃料改質器１８
（リフォーマー）にて改質して得られる水素含有改質ガ
スから、さらに水素ガスのみを効率よく選択的に吸蔵す
るためのタンクであって、比較的簡単な内部構造とす
る。その理由は、このタンクの役割に拠るのであって、
このタンクの場合、硫黄や一酸化炭素による水素吸蔵合
金の被毒をある程度予測した上で、吸蔵の速さに拘泥す
ることなく、むしろ効率よく水素ガスの吸蔵が起こるよ
うにすることが必要であって、そのためには水素回収率
と貯蔵量の増大に適合させるべく簡単な構造にしなけれ
ばならないからである。もっとも、本発明の水素回収・
貯蔵容器は、水素吸蔵タンク２０としてだけでなく、水
素放出タンク２１としても用いることができる。さらに
は、燃料改質器１８の運転中に余剰水素が発生した場合
に、当該余剰水素をタイミング良くこれらのタンク２
０，２１に吸蔵することができる。In the present invention, the above-mentioned hydrogen recovery / storage container is used as a hydrogen storage tank 20 of a fuel cell system as shown in FIG. By the way, in a general hydrogen supply device, the storage tank 20 is provided with a fuel gas such as natural gas, methanol, mesa, coal, etc.
It is a tank for efficiently and selectively storing only hydrogen gas from the hydrogen-containing reformed gas obtained by reforming in the (reformer), and has a relatively simple internal structure. The reason is because of the role of this tank,
In the case of this tank, it is necessary to predict the poisoning of the hydrogen storage alloy by sulfur and carbon monoxide to some extent, and to ensure that hydrogen gas is stored efficiently without being bound by the speed of storage. This is because, for this purpose, a simple structure must be adopted in order to adapt to the increase in the hydrogen recovery rate and the storage amount. However, the hydrogen recovery and
The storage container can be used not only as the hydrogen storage tank 20 but also as the hydrogen release tank 21. Further, when surplus hydrogen is generated during the operation of the fuel reformer 18, the surplus hydrogen is supplied to these tanks 2 in a timely manner.
It can be stored at 0,21.
【００１４】次に、上述した燃料電池システムの作動方
法について図６及び図７に基づいて説明する。 通常運転プロセス（改質運転状態） この状態は、燃料改質器１８から発生する通常の水素含
有改質ガスを、まず吸蔵タンク２０を経由させることな
く燃料電池１９の燃料として直接使用する他、吸蔵タン
ク２０には前記改質ガス中に含まれる水素のみを選択的
に吸蔵させる。そして、運転停止の前などにこの吸蔵タ
ンク２０に吸蔵した水素を、燃料電池１９ではなく放出
タンク２１に供給してそこに貯蔵するプロセスである。
即ち、放出タンク２１に吸蔵する場合、図７に示すよう
に、燃料改質器１８から吸蔵タンク２０に向かうライン
のバルブＶ１および吸蔵タンク２０から燃料電池１９へ
と向かうラインのバルブＶ２，Ｖ４を開とし、水素含有
改質ガスを導入すると同時に、２５℃の冷水を供給する
ことにより、吸蔵タンク２０の内部の水素吸蔵合金に水
素を吸蔵する。そして、主として、燃料電池１９の停止
の前に、前記バルブＶ１，Ｖ４を閉じると共に吸蔵タン
ク２０と放出タンク２１との間に介挿してあるバルブＶ
２，Ｖ３を開として、吸蔵タンク２０に６０℃の温水を
供給して充填した水素吸蔵合金に貯蔵してある高純度の
水素ガスを、発生させ、これを放出タンク２１に移送す
る。このとき、放出タンク２１内には水素ガス吸蔵のた
めに冷水（２０℃程度）を供給してこれを冷却する。Next, an operation method of the above-described fuel cell system will be described with reference to FIGS. Normal operation process (reforming operation state) In this state, a normal hydrogen-containing reformed gas generated from the fuel reformer 18 is used directly as fuel for the fuel cell 19 without first passing through the storage tank 20. The storage tank 20 selectively stores only hydrogen contained in the reformed gas. This is a process in which the hydrogen stored in the storage tank 20 before the operation is stopped is supplied to the discharge tank 21 instead of the fuel cell 19 and stored therein.
That is, when storing in the discharge tank 21, as shown in FIG. 7, the valves V1 and V4 on the line from the fuel reformer 18 to the storage tank 20 and the valves V2 and V4 on the line from the storage tank 20 to the fuel cell 19 are connected. When the hydrogen storage alloy is opened and hydrogen-containing reformed gas is introduced, at the same time as supplying cold water at 25 ° C., hydrogen is stored in the hydrogen storage alloy in the storage tank 20. Before stopping the fuel cell 19, the valves V1 and V4 are closed and the valve V inserted between the storage tank 20 and the discharge tank 21 is mainly inserted.
2. When V3 is opened, hot water at 60 ° C. is supplied to the storage tank 20 to generate high-purity hydrogen gas stored in the filled hydrogen storage alloy, and this is transferred to the discharge tank 21. At this time, cold water (about 20 ° C.) is supplied into the discharge tank 21 for storing hydrogen gas and is cooled.
【００１５】始動運転プロセス（改質運転停止状態） この状態は、燃料改質器１８の停止時において、燃料電
池を起動させる時のプロセスである。このときは改質ガ
スが得られないので、上述した放出タンク２１に貯蔵し
た高純度の水素ガスを高速度で放出させることで対処す
る。そのために、燃料改質器１８から貯蔵タンク２０の
出口までのバルブＶ１，Ｖ２を閉じ、放出タンク２１か
ら燃料電池１９に向かうバルブＶ３，Ｖ４を開として、
該タンク内に６０℃程度の温水を供給して、吸蔵室内に
充填した水素吸蔵合金から水素を発生させ、この水素を
燃料電池１９に供給する。そして、燃料電池システムが
起動し、前記燃料改質器１８の運転が再開された後は、
先の定常運転プロセスに戻ることになる。Start Operation Process (Reforming Operation Stop State) This state is a process for starting the fuel cell when the fuel reformer 18 is stopped. In this case, since no reformed gas is obtained, the high-purity hydrogen gas stored in the release tank 21 described above is released at a high speed. For this purpose, the valves V1 and V2 from the fuel reformer 18 to the outlet of the storage tank 20 are closed, and the valves V3 and V4 from the discharge tank 21 to the fuel cell 19 are opened.
Hot water of about 60 ° C. is supplied into the tank to generate hydrogen from the hydrogen storage alloy filled in the storage chamber, and this hydrogen is supplied to the fuel cell 19. Then, after the fuel cell system is started and the operation of the fuel reformer 18 is restarted,
It will return to the previous steady operation process.
【００１６】[0016]
【発明の効果】本発明の水素回収・貯蔵容器は、水素吸
蔵合金が結着剤により固定されているために、水素吸蔵
合金粉末の微粉化による脱落が防止される。また、移動
体用としての使用においても振動による水素吸蔵合金粉
末の偏りを生じないので、反応容器内の圧力損失を一定
にすることが可能となり制御が容易となる。さらに、本
発明の水素回収・貯蔵容器は熱伝導が良く急速吸蔵・放
出が可能であり、これを燃料電池システムに適用した場
合には、燃料電池にすばやい水素供給ができ、とりわけ
始動、高出力運転時の応答性能が格段に優れるという効
果が得られる。According to the hydrogen recovery / storage container of the present invention, since the hydrogen storage alloy is fixed by the binder, the hydrogen storage alloy powder is prevented from falling off due to pulverization. Further, even when the hydrogen storage alloy powder is used for a moving body, the bias of the hydrogen storage alloy powder due to vibration does not occur, so that the pressure loss in the reaction vessel can be made constant and control becomes easy. Furthermore, the hydrogen recovery / storage container of the present invention has good heat conduction and is capable of quick occlusion / release, and when this is applied to a fuel cell system, it can quickly supply hydrogen to the fuel cell, and particularly when starting and outputting high power. The effect that the response performance at the time of driving is remarkably excellent is obtained.
【図１】本発明における水素吸蔵性シートを巻回積層し
た状態を説明するための図である。FIG. 1 is a diagram for explaining a state in which a hydrogen storage sheet according to the present invention is wound and laminated.
【図２】本発明における平板状の水素吸蔵性シートの積
層状態を説明するための図である。FIG. 2 is a view for explaining a state of lamination of a flat hydrogen storage sheet in the present invention.
【図３】本発明に係る水素回収・貯蔵容器（円筒状積層
シート使用）の一例を示す断面透視図である。FIG. 3 is a cross-sectional perspective view showing an example of a hydrogen recovery / storage container (using a cylindrical laminated sheet) according to the present invention.
【図４】本発明に係る水素回収・貯蔵容器（円筒状積層
シート使用）の他の一例を示す断面透視図である。FIG. 4 is a cross-sectional perspective view showing another example of the hydrogen recovery / storage container (using a cylindrical laminated sheet) according to the present invention.
【図５】本発明に係る水素回収・貯蔵容器（平板状積層
シート使用）の一例を説明するための図である。FIG. 5 is a view for explaining an example of a hydrogen recovery / storage container (using a flat laminated sheet) according to the present invention.
【図６】燃料電池システムのフローを示す説明図であ
る。FIG. 6 is an explanatory diagram showing a flow of the fuel cell system.
【図７】燃料電池システムに本発明装置を用いたときの
作動を説明するための図である。FIG. 7 is a diagram for explaining an operation when the device of the present invention is used in a fuel cell system.
１： 水素吸蔵性シート ２： 円筒状積層シート ３： 円筒内管 ４，４’： ガスの導入・放出口 ５： 平板状積層シート ６： 箱型密閉容器 ７，７’： ガスの導入・放出口 ８： 密閉容器 ９，９’： ガス導入・放出管 １０，１０’： ガスヘッダー １１： パイプ １２，１２’： 熱媒用導入・放出管 １３： 密閉容器 １４： 平板状の水素吸蔵性シートの積層体 １５，１５’： ガス導入・放出管 １６： 熱媒管 １８： 燃料改質器 １９： 燃料電池 ２０： 水素吸蔵タンク ２１： 水素放出タンク 1: Hydrogen storage sheet 2: Cylindrical laminated sheet 3: Cylindrical inner tube 4, 4 ': Gas introduction / discharge port 5: Flat laminated sheet 6: Box-shaped closed container 7, 7': Gas introduction / discharge Outlet 8: Closed container 9, 9 ': Gas introduction / discharge tube 10, 10': Gas header 11: Pipe 12, 12 ': Heat medium introduction / discharge tube 13: Closed container 14: Flat hydrogen absorbing sheet Laminate 15, 15 ': gas introduction / discharge tube 16: heating medium tube 18: fuel reformer 19: fuel cell 20: hydrogen storage tank 21: hydrogen release tank
───────────────────────────────────────────────────── フロントページの続き (72)発明者 高橋 昌志 茨城県つくば市東光台５丁目９番地６ 日 本重化学工業株式会社筑波研究所内 (72)発明者 内田 浩司 茨城県つくば市東光台５丁目９番地６ 日 本重化学工業株式会社筑波研究所内 (72)発明者 小林 賢一 茨城県つくば市東光台５丁目９番地６ 日 本重化学工業株式会社筑波研究所内 (72)発明者 縫谷 芳雄 埼玉県和光市中央１丁目４番１号 株式会 社本田技術研究所内 (72)発明者 佐保田 克三 埼玉県和光市中央１丁目４番１号 株式会 社本田技術研究所内 Ｆターム(参考） 4G040 AA24 AA33 FC02 FD04 FE01 5H027 AA02 BA01 BA14 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Masashi Takahashi 5-9-9 Tokodai, Tsukuba, Tsukuba, Ibaraki, Japan Tsukuba Research Laboratories (72) Inventor Koji Uchida 5-9, Tokodai, Tsukuba, Ibaraki No. 6 Nihon Heavy Chemical Industry Co., Ltd., Tsukuba Research Laboratories (72) Inventor Kenichi Kobayashi 5-9-9 Tokodai, Tsukuba City, Ibaraki Pref. 1-4-1, Chuo Inside Honda R & D Co., Ltd. (72) Inventor Katsuzo Sabota 1-4-1, Chuo, Wako-shi, Saitama F-term inside Honda R & D Co., Ltd. 4G040 AA24 AA33 FC02 FD04 FE01 5H027 AA02 BA01 BA14
Claims (8)
状とし、金属多孔質体シートに塗布又は充填した後、加
圧成形した水素吸蔵性シートを積層して、ガス入り口と
ガス出口とを備えた容器内に収納してなることを特徴と
する水素回収・貯蔵容器。The present invention relates to a method of forming a paste into a paste by adding a binder to a hydrogen-absorbing alloy, applying or filling a porous metal sheet, and laminating a pressure-formed hydrogen-absorbing sheet. A hydrogen recovery / storage container which is housed in a container provided with:
シートを重ねて張り合わせ積層したことからなることを
特徴とする請求項１に記載の水素回収・貯蔵容器。2. The hydrogen recovery / storage container according to claim 1, wherein a porous sheet is further laminated on the hydrogen storage sheet and laminated.
シートと重ね合せて巻回したことからなることを特徴と
する請求項１に記載の水素回収・貯蔵容器。3. The hydrogen recovery / storage container according to claim 1, wherein the hydrogen storage sheet is further wound by overlapping with a porous sheet.
シートと重ね合せて巻回して得られた筒状体を、長手方
向に分割した後、その分割体を複数個並べて容器内に収
納してなることを特徴とする請求項１に記載の水素回収
・貯蔵容器。4. A tubular body obtained by laminating the hydrogen-absorbing sheet on a porous sheet and winding it is divided in the longitudinal direction, and a plurality of the divided bodies are arranged in a container. The hydrogen recovery / storage container according to claim 1, wherein:
るいは並列に配置したことを特徴とする請求項１〜４の
いずれか一項に記載の水素回収貯蔵装置。5. The hydrogen recovery and storage device according to claim 1, wherein a plurality of hydrogen recovery and storage containers are arranged in series or in parallel.
ヘッダーを備えた密閉容器内に、水素吸蔵性シートを巻
回して収納してある筒状内管が複数個並設されており、
該筒状内管は上下のガスヘッダーに連結していると共
に、密閉容器内の空隙部には熱媒体を流入するように形
成されていることを特徴とする請求項１及び請求項３〜
５のいずれか一項に記載の水素回収・貯蔵容器。6. A sealed container having a gas inlet and a gas outlet and provided with a gas header is provided with a plurality of tubular inner tubes in which a hydrogen storage sheet is wound and stored. ,
The tubular inner pipe is connected to upper and lower gas headers, and is formed so as to allow a heat medium to flow into a gap in the closed vessel.
6. The hydrogen recovery / storage container according to any one of items 5 to 5.
内に、平板状からなる請求項１記載の水素吸蔵性シート
を複数枚積層して収納されていると共に、該シートと密
閉容器側面とを貫通して熱媒体用の流入管が複数本並設
されていることを特徴とする請求項１，２及び５のいず
れか一項に記載の水素回収・貯蔵容器。7. A plurality of flat sheets of the hydrogen-absorbing sheet according to claim 1, which are stored in a sealed container having a gas inlet and a gas outlet, and the sheet and the side surface of the sealed container. The hydrogen recovery / storage container according to any one of claims 1, 2, and 5, wherein a plurality of heat medium inflow pipes are arranged in parallel with each other.
置の運転中に生成する改質ガス中に含まれる水素を選択
的に吸蔵し、また、吸蔵した水素を放出タンクに供給す
るために用いられることを特徴とする請求項１〜７のい
ずれか一項に記載の燃料電池用水素回収・貯蔵容器。8. The hydrogen recovery / storage container selectively stores hydrogen contained in reformed gas generated during operation of the fuel reformer and supplies the stored hydrogen to a discharge tank. The hydrogen recovery / storage container for a fuel cell according to any one of claims 1 to 7, which is used for:
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2000049541A JP4663839B2 (en) | 2000-02-25 | 2000-02-25 | Hydrogen recovery / storage container |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2000049541A JP4663839B2 (en) | 2000-02-25 | 2000-02-25 | Hydrogen recovery / storage container |
Publications (3)
| Publication Number | Publication Date |
|---|---|
| JP2001241599A true JP2001241599A (en) | 2001-09-07 |
| JP2001241599A5 JP2001241599A5 (en) | 2006-12-07 |
| JP4663839B2 JP4663839B2 (en) | 2011-04-06 |
Family
ID=18571465
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2000049541A Expired - Fee Related JP4663839B2 (en) | 2000-02-25 | 2000-02-25 | Hydrogen recovery / storage container |
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| Country | Link |
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Cited By (9)
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| JP2009120435A (en) * | 2007-11-14 | 2009-06-04 | Toyota Motor Corp | Filter device for removing impurities from hydrogen gas |
| JP2010248037A (en) * | 2009-04-16 | 2010-11-04 | Kobe Steel Ltd | Hydrogen purification method and reaction vessel for hydrogen-storage alloy |
| US7875107B2 (en) | 2007-06-19 | 2011-01-25 | Toyota Jidosha Kabushiki Kaisha | Hydrogen storage tank and its manufacturing method |
| WO2019026872A1 (en) * | 2017-07-31 | 2019-02-07 | 株式会社Ａｔｏｍｉｓ | Gas storage container |
| CN114962989A (en) * | 2022-06-20 | 2022-08-30 | 樊品良 | Hydrogen oil-free water purification pressurization system |
| CN115574258A (en) * | 2022-09-22 | 2023-01-06 | 上海镁源动力科技有限公司 | Solid-state hydrogen storage and discharge components and solid-state hydrogen discharge system using gas circulation heating |
| KR20230129072A (en) * | 2022-02-28 | 2023-09-06 | 한국에너지기술연구원 | Hydrogen production and storage systems |
| USD1025284S1 (en) | 2020-10-15 | 2024-04-30 | Atomis Inc. | Gas storage container |
| CN119554163A (en) * | 2024-12-03 | 2025-03-04 | 南京岳家军氢电科技发展有限公司 | High-efficiency methanol reforming hydrogen production ship power system and method |
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| CN114962989B (en) * | 2022-06-20 | 2024-04-05 | 樊品良 | Hydrogen oil-free water purification pressurization system |
| CN114962989A (en) * | 2022-06-20 | 2022-08-30 | 樊品良 | Hydrogen oil-free water purification pressurization system |
| CN115574258A (en) * | 2022-09-22 | 2023-01-06 | 上海镁源动力科技有限公司 | Solid-state hydrogen storage and discharge components and solid-state hydrogen discharge system using gas circulation heating |
| CN119554163A (en) * | 2024-12-03 | 2025-03-04 | 南京岳家军氢电科技发展有限公司 | High-efficiency methanol reforming hydrogen production ship power system and method |
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|---|---|
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