JP2003154260A - Gas storage material - Google Patents
Gas storage materialInfo
- Publication number
- JP2003154260A JP2003154260A JP2001355848A JP2001355848A JP2003154260A JP 2003154260 A JP2003154260 A JP 2003154260A JP 2001355848 A JP2001355848 A JP 2001355848A JP 2001355848 A JP2001355848 A JP 2001355848A JP 2003154260 A JP2003154260 A JP 2003154260A
- Authority
- JP
- Japan
- Prior art keywords
- gas
- hydrogen
- storage material
- gas storage
- cnts
- 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.)
- Pending
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
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、ガス吸蔵材に関す
るものである。TECHNICAL FIELD The present invention relates to a gas storage material.
【０００２】[0002]
【従来の技術】ガスの吸蔵材としては、各種のものが知
られている。例えば、水素吸蔵材としては水素ガスを吸
蔵する各種の金属水素化物を用いる水素吸蔵合金が知ら
れ、水素自動車等での利用を目指して開発が進められて
いる。水素吸蔵合金の水素吸蔵量は水素吸蔵合金に対す
る重量比では約１．０重量％である。水素吸蔵合金は大
型の水素ボンベによる輸送コストと大差ないのが現状で
ある。現状の１．５倍〜２倍の水素吸蔵量を持つ合金の
開発が目標とされている。水素吸蔵合金の最大の問題点
として、密度が大きいことと、水素の吸蔵と放出とを繰
り返すうちに劣化することが上げられる。これらの問題
点を克服するものとして炭素系材料が注目さている。活
性炭や微細なグラファイトが積層した構造のｎｍサイズ
の炭素繊維、多層カーボンナノチューブ、単層カーボン
ナノチューブなどが検討されてきた。これらの中には極
めて大きな水素吸蔵能力を示すと報告されたものもあ
る。理論的な研究から、単層カーボンナノチューブが最
も可能性が高いとの評価が定着しつつある。しかし、単
層カーボンナノチューブでも、その水素吸蔵量の現状は
１〜３重量％と低い。2. Description of the Related Art Various gas storage materials are known. For example, as a hydrogen storage material, hydrogen storage alloys using various metal hydrides that store hydrogen gas are known, and their development is being promoted with the aim of use in hydrogen automobiles and the like. The hydrogen storage amount of the hydrogen storage alloy is about 1.0% by weight relative to the hydrogen storage alloy. Currently, hydrogen storage alloys are not much different from the transportation costs of large hydrogen cylinders. The goal is to develop an alloy that has a hydrogen storage capacity that is 1.5 to 2 times the current level. The biggest problems with hydrogen storage alloys are that they have a high density and that they deteriorate during repeated storage and release of hydrogen. Carbon-based materials are attracting attention as a means of overcoming these problems. Nm-sized carbon fibers having a structure in which activated carbon and fine graphite are laminated, multi-walled carbon nanotubes, single-walled carbon nanotubes, and the like have been studied. Some of these have been reported to show extremely high hydrogen storage capacity. From theoretical studies, it is becoming clear that single-walled carbon nanotubes are the most likely. However, even with single-walled carbon nanotubes, the present hydrogen storage capacity is as low as 1 to 3% by weight.
【０００３】[0003]
【発明が解決しようとする課題】本発明は、高められた
ガス吸蔵量を有するガス吸蔵材を提供することをその課
題とする。SUMMARY OF THE INVENTION An object of the present invention is to provide a gas storage material having an increased gas storage amount.
【０００４】[0004]
【課題を解決するための手段】本発明者らは、前記課題
を解決すべく鋭意研究を重ねた結果、本発明を完成する
に至った。即ち、本発明によれば、以下に示すガス吸蔵
材及び水素吸蔵物が提供される。
（１）少なくとも一方の端部が開口しているカーボンナ
ノチューブにおいて、該開口がガス吸着性材料によって
封止されているカーボンナノチューブからなることを特
徴とするガス吸蔵材。
（２）該ガス吸着性材料が、水素吸着性金属である前記
（１）に記載のガス吸蔵材。
（３）該ガス吸着性材料が、高分子材料である前記
（１）に記載のガス吸蔵材。
（４）前記（２）に記載のガス吸蔵材に対して水素を吸
蔵させてなる水素吸蔵物。The present inventors have completed the present invention as a result of intensive studies to solve the above problems. That is, according to the present invention, the following gas storage material and hydrogen storage material are provided. (1) A gas storage material, wherein at least one end of the carbon nanotube is open, and the opening is made of a carbon nanotube sealed with a gas adsorbent material. (2) The gas storage material according to (1), wherein the gas adsorbent material is a hydrogen adsorbent metal. (3) The gas storage material according to (1), wherein the gas adsorbent material is a polymer material. (4) A hydrogen storage material obtained by storing hydrogen in the gas storage material according to (2).
【０００５】[0005]
【発明の実施の形態】本発明のガス吸蔵材用材料として
用いるカーボンナノチューブ（以下、単にＣＮＴｓとも
言う）は、その一方の端部又は両方の端部が開口してい
るものである。そのＣＮＴｓは、単層又は多層のもので
あることができる。このＣＮＴｓにおいて、その内径
は、０．４〜５０ｎｍ、好ましくは１〜１０ｎｍ、より
好ましくは１〜５ｎｍである。その長さは、０．０１〜
１０μｍ、好ましくは０．１〜１μｍである。一般的に
は、ＣＮＴｓの生成時の長さと内径との比（アスペクト
比）は５００〜５０００程度であるが、本発明の場合、
ボールミル等を用いて切断して、そのアスペクト比を１
０〜５００、好ましくは５０〜２００程度に調節するの
が好ましい。BEST MODE FOR CARRYING OUT THE INVENTION Carbon nanotubes (hereinafter, also simply referred to as CNTs) used as a material for a gas storage material of the present invention have one end or both ends opened. The CNTs can be single or multi-layered. In the CNTs, the inner diameter is 0.4 to 50 nm, preferably 1 to 10 nm, more preferably 1 to 5 nm. Its length is 0.01 ~
The thickness is 10 μm, preferably 0.1 to 1 μm. Generally, the ratio of the length to the inner diameter (aspect ratio) at the time of producing CNTs is about 500 to 5000, but in the case of the present invention,
Cut with a ball mill etc. and set the aspect ratio to 1
It is preferably adjusted to 0 to 500, preferably about 50 to 200.
【０００６】前記のようなＣＮＴｓは、従来公知のもの
であり、各種の方法で製造することができる。このよう
な方法としては、アーク放電法、レーザー法、炭化水素
を触媒下で熱分解する方法等が挙げられる。このような
ＣＮＴｓの製造方法においては、通常、両端が閉じた多
層又は単層のＣＮＴｓが生成される。これらの方法の
内、炭化水素の触媒下での熱分解法における多層のＣＮ
Ｔｓの先端部には触媒金属があり、その触媒金属の先端
は炭素で覆われている。これらのＣＮＴｓ先端の炭素
は、空気中で４００〜６００度の温度で酸化処理する方
法等によって、一方の端部が開口したものやその両端部
が開口したもの等が生成される。前述のボールミル等を
用いてＣＮＴｓを切断する方法も端部を開口する有効な
手段となる。本発明のガス吸蔵材は、ＣＮＴｓの開口を
封止材により封止した構造を有する。The above-mentioned CNTs are conventionally known and can be manufactured by various methods. Examples of such a method include an arc discharge method, a laser method, and a method of thermally decomposing hydrocarbons in the presence of a catalyst. In such a method for producing CNTs, usually, multi-layered or single-layered CNTs having both ends closed are produced. Among these methods, multilayer CN in the pyrolysis method under the catalyst of hydrocarbon
There is a catalytic metal at the tip of Ts, and the tip of the catalytic metal is covered with carbon. The carbon at the tip of these CNTs is produced with one end opened or both ends opened by a method such as oxidation treatment in air at a temperature of 400 to 600 degrees. The method of cutting the CNTs by using the above-described ball mill or the like is also an effective means for opening the ends. The gas storage material of the present invention has a structure in which the openings of CNTs are sealed with a sealing material.
【０００７】本発明においては、前記開口封止材として
は、吸蔵すべき対象ガスに対しガス吸着性を有する材料
（ガス吸着性材料）を用いる。このガス吸着性材料は、
金属（合金を含む）、高分子物質等であることができ
る。In the present invention, as the opening sealing material, a material having a gas adsorbing property for the target gas to be stored (gas adsorbing material) is used. This gas adsorbent material is
It can be a metal (including alloy), a polymeric substance, or the like.
【０００８】本発明で用いる好ましいガス吸着性材料
は、水素ガス吸着性材料である。このようなものには、
水素吸蔵合金等として知られている各種の金属や金属水
素化物等が包含される。金属水素化物を形成する金属と
しては、Ｐｔ、Ｐｄ、Ｎｉ、Ｃｏ、Ｃａ、Ｍｇ、Ｌａ、
Ｓｍ、Ｔｉ、Ｚｒ、Ｖ、Ｎｂ、合金としてはＴｉ／Ｆ
ｅ、Ｌａ／Ｎｉ、Ｍｇ／Ｎｉ、Ｃａ／Ｎｉ等が挙げられ
る。本発明で好ましく用いる水素吸蔵合金及びその水素
化物を示すと、ＬａＮｉ5（ＬａＮｉ5Ｈ5.0）、ＴｉＦ
ｅ（ＴｉＦｅＨ1.9）、Ｍｇ2Ｎｉ（Ｍｇ2ＮｉＨ4.0）、
ＣａＮｉ5（ＣａＮｉ5Ｈ5.0）等が挙げられる。The preferred gas adsorbent material for use in the present invention is a hydrogen gas adsorbent material. Something like this
Various metals and metal hydrides known as hydrogen storage alloys are included. As the metal forming the metal hydride, Pt, Pd, Ni, Co, Ca, Mg, La,
Sm, Ti, Zr, V, Nb, Ti / F as alloy
e, La / Ni, Mg / Ni, Ca / Ni and the like. The hydrogen storage alloys and their hydrides preferably used in the present invention are shown as LaNi 5 (LaNi 5 H 5.0 ) and TiF.
e (TiFeH 1.9 ), Mg 2 Ni (Mg 2 NiH 4.0 ),
CaNi 5 (CaNi 5 H 5.0), and the like.
【０００９】本発明で用いる他の好ましいガス吸着性材
料は、高分子物質である。このようなものには、ガス分
離膜に用いられるポリイミド、酢酸セルロース、ポリエ
チレン、ポリスチレン、ポリ塩化ビニール、ポリフッ化
ビニールなどがよく知られている。Another preferred gas adsorbent material for use in the present invention is a polymeric material. Well-known examples of such materials include polyimide, cellulose acetate, polyethylene, polystyrene, polyvinyl chloride, and polyvinyl fluoride used for gas separation membranes.
【００１０】前記ポリイミドや酢酸セルロースは、
Ｈ2、Ｈｅ、ＣＯ2、メタンやエタン、プロピレン等の炭
素数１〜３の低級炭化水素ガスに対して吸着性を示す
他、ＣＯ、Ｎ2、Ｏ2等に対しても吸着性を示す。The above-mentioned polyimide and cellulose acetate are
In addition to having adsorptivity for H 2 , He, CO 2 , lower hydrocarbon gas having 1 to 3 carbon atoms such as methane, ethane, propylene, etc., it also has adsorptivity for CO, N 2 , O 2, etc. .
【００１１】ポリエチレン、ポリスチレン、ポリ塩化ビ
ニル、ポリフッ化ビニールは、Ｈ2に対して吸着性を示
す他、ＣＯ等に対しても吸着性を示す。Polyethylene, polystyrene, polyvinyl chloride, and polyvinyl fluoride show adsorptivity to H 2 as well as CO and the like.
【００１２】ＣＮＴｓの開口端を封止材で封止する方法
としては、各種の方法を用いることができる。このよう
な方法としては、例えば、以下の方法を示すことができ
る。
（ｉ）炭化水素の触媒下での熱分解法における多層のＣ
ＮＴｓの先端には触媒金属があり、触媒金属の先端は炭
素で覆われている。このＣＮＴｓ先端の炭素を空気中で
４００〜６００度の温度で酸化処理する方法等によって
触媒金属を露出させて金属封止された開口を有するＣＮ
Ｔｓを形成する方法。
（ii）アーク放電法やレーザー法、炭化水素の触媒によ
る熱分解法などで合成された多層又は単層のＣＮＴｓ先
端の炭素を空気中で４００〜６００度の温度で酸化処理
する方法やＣＮＴｓをボールミルで切断する方法等によ
って端部を開口させ、この開口端部に金属、高分子物質
等の封止剤を蒸着する方法。
（iii）アーク放電法やレーザー法、炭化水素の触媒に
よる熱分解法等で合成された多層又は単層のＣＮＴｓ先
端の炭素を空気中で４００〜６００度の温度で酸化処理
する方法や酸を用いる湿式酸化方法、ボールミルで切断
する方法などによって端部を開口させ、この端が開口し
たＣＮＴｓを金属塩の酸溶液に浸す等の方法。Various methods can be used to seal the open ends of the CNTs with a sealing material. As such a method, for example, the following method can be shown. (I) Multi-layered C in the thermal decomposition process of hydrocarbons
There is a catalytic metal at the tip of NTs, and the tip of the catalytic metal is covered with carbon. CN having an opening that is metal-sealed by exposing the catalytic metal by a method of oxidizing carbon at the tip of the CNTs in air at a temperature of 400 to 600 degrees
Method of forming Ts. (Ii) Multi-layered or single-layered CNTs synthesized by an arc discharge method, a laser method, a thermal decomposition method using a hydrocarbon catalyst, or the like. A method in which an end is opened by a method such as cutting with a ball mill, and a sealant such as a metal or a polymer substance is vapor-deposited on the open end. (Iii) A method of oxidizing carbon at the tip of multi-layered or single-layered CNTs synthesized by an arc discharge method, a laser method, a thermal decomposition method using a hydrocarbon catalyst, or the like in air at a temperature of 400 to 600 ° C. or an acid. A method in which the end portion is opened by a wet oxidation method used, a method of cutting with a ball mill, or the like, and the CNTs having the opened end portion are immersed in an acid solution of a metal salt.
【００１３】本発明のガス吸蔵材は、これを吸蔵すべき
対象ガスと接触させることにより、そのＣＮＴｓ内部に
そのガス吸蔵させることができる。このガス吸蔵の機構
を水素の吸蔵を例にとって示すと以下の通りである。水
素吸着性材料で開口端が封止されたＣＮＴｓを水素ガス
と接触させると、その水素ガスは、先ず、開口端を封止
する材料内に吸着（吸蔵）される。この材料内に吸着さ
れた水素は、その材料内を拡散して、チューブ内空間に
対向する側の材料端面に達する。この場合、その材料端
面の水素濃度は、チューブ内空間の水素濃度より大き
く、この水素濃度差を推進力として、その材料端面の水
素は離脱してチューブ内に拡散侵入する。チューブ内空
間の水素は、そのチューブ内壁面に吸着され、これによ
ってチューブ内水素濃度は低く保持され、その結果、チ
ューブ内空間にはその封止材料を介して水素が連続的に
拡散侵入する。このようにして、チューブ壁には水素が
多分子吸着され、その吸着量が飽和吸着量に達する。こ
のようにして本発明のガス吸蔵材には多量（３重量％以
上）の水素を吸蔵させることができる。The gas storage material of the present invention can be stored inside the CNTs by bringing it into contact with the target gas to be stored. The mechanism of this gas occlusion will be described below by taking the occlusion of hydrogen as an example. When CNTs whose opening ends are sealed with a hydrogen adsorbing material are brought into contact with hydrogen gas, the hydrogen gas is first adsorbed (occluded) in the material that seals the opening ends. The hydrogen adsorbed in this material diffuses in the material and reaches the end surface of the material on the side facing the inner space of the tube. In this case, the hydrogen concentration on the material end surface is higher than the hydrogen concentration in the tube inner space, and the hydrogen on the material end surface is released and diffuses into the tube by using this hydrogen concentration difference as a driving force. Hydrogen in the tube inner space is adsorbed on the inner wall surface of the tube, whereby the hydrogen concentration in the tube is kept low, and as a result, hydrogen continuously diffuses and enters the tube inner space through the sealing material. In this way, multiple molecules of hydrogen are adsorbed on the tube wall, and the adsorbed amount reaches the saturated adsorbed amount. In this way, the gas storage material of the present invention can store a large amount (3% by weight or more) of hydrogen.
【００１４】本発明のガス吸蔵材と対象ガスとの接触方
法としては、ガス吸蔵材を充填した充填塔に対して、対
象ガスを流通接触させる方法や、攪拌装置内において対
象ガスの流通下でガス吸蔵材を攪拌する方法、流動化用
ガスとして対象ガスを用いて、ガス吸蔵材を流動化させ
る方法等の従来公知の各種の固体／気体接触法を用いる
ことができる。The method for contacting the gas storage material of the present invention with the target gas may be a method of bringing the target gas into flow contact with a packed column filled with the gas storage material, or a method of contacting the target gas in a stirrer under the flow of the target gas. Various conventionally known solid / gas contact methods such as a method of stirring the gas storage material and a method of fluidizing the gas storage material by using the target gas as the fluidizing gas can be used.
【００１５】[0015]
【発明の効果】本発明のガス吸蔵材は、そのカーボンナ
ノチューブ内壁面のすぐれたガス吸着性により、多量の
対象ガスを吸蔵することができる。この場合、その開口
端部を封止する材料として、特定のガスに対して選択吸
着性を有する材料を用いることにより、混合ガス中から
特定のガスを選択的に吸蔵させることができる。本発明
による開口端を水素吸着性材料で封止したガス吸蔵材
は、水素吸蔵材として好適のものである。このような水
素吸蔵材には、３重量％以上、好ましくは５重量％以上
の水素を吸蔵させることができる。その吸蔵量の上限値
は、通常１０重量％程度である。The gas storage material of the present invention can store a large amount of target gas due to its excellent gas adsorption property on the inner wall surface of the carbon nanotube. In this case, by using a material having a selective adsorption property for a specific gas as a material for sealing the opening end, the specific gas can be selectively occluded from the mixed gas. The gas storage material having the open end sealed with a hydrogen adsorbing material according to the present invention is suitable as a hydrogen storage material. Such hydrogen storage material can store 3% by weight or more, preferably 5% by weight or more of hydrogen. The upper limit of the storage amount is usually about 10% by weight.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 内田 邦夫 茨城県つくば市東１−１−１ 独立行政法 人産業技術総合研究所 つくばセンター内 Ｆターム(参考） 4G040 AA01 AA32 4G046 CB01 CB08 4G066 AA02B AA02D AA04B AC13B AC27B AC27D CA38 ─────────────────────────────────────────────────── ─── Continued front page (72) Inventor Kunio Uchida 1-1-1 Higashi 1-1-1 Tsukuba City, Ibaraki Prefecture National Institute of Advanced Industrial Science and Technology Tsukuba Center F-term (reference) 4G040 AA01 AA32 4G046 CB01 CB08 4G066 AA02B AA02D AA04B AC13B AC27B AC27D CA38
Claims (4)
ーボンナノチューブにおいて、該開口がガス吸着性材料
によって封止されているカーボンナノチューブからなる
ことを特徴とするガス吸蔵材。1. A gas storage material, wherein at least one end of the carbon nanotube is open, and the opening is made of a carbon nanotube sealed with a gas adsorbing material.
ある請求項１に記載のガス吸蔵材。2. The gas storage material according to claim 1, wherein the gas adsorbent material is a hydrogen adsorbent metal.
請求項１に記載のガス吸蔵材。3. The gas storage material according to claim 1, wherein the gas adsorbent material is a polymer material.
素を吸蔵させてなる水素吸蔵物。4. A hydrogen storage material obtained by storing hydrogen in the gas storage material according to claim 2.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2001355848A JP2003154260A (en) | 2001-11-21 | 2001-11-21 | Gas storage material |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2001355848A JP2003154260A (en) | 2001-11-21 | 2001-11-21 | Gas storage material |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JP2003154260A true JP2003154260A (en) | 2003-05-27 |
Family
ID=19167475
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2001355848A Pending JP2003154260A (en) | 2001-11-21 | 2001-11-21 | Gas storage material |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2003154260A (en) |
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2004261739A (en) * | 2003-03-03 | 2004-09-24 | Toyota Motor Corp | Hydrogen occlusion composite material |
| JP2006007127A (en) * | 2004-06-28 | 2006-01-12 | Shimadzu Corp | Adsorbent and adsorbing method by using fibrous carbon |
| WO2007004652A1 (en) * | 2005-07-05 | 2007-01-11 | National University Corporation NARA Institute of Science and Technology | Method for producing carbon nanotube dispersion liquid |
| WO2007007594A1 (en) * | 2005-07-11 | 2007-01-18 | National University Corporation NARA Institute of Science and Technology | Process for preparation of aqueous solution containing carbon nanotube |
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| WO2007004652A1 (en) * | 2005-07-05 | 2007-01-11 | National University Corporation NARA Institute of Science and Technology | Method for producing carbon nanotube dispersion liquid |
| JP5109129B2 (en) * | 2005-07-05 | 2012-12-26 | 国立大学法人 奈良先端科学技術大学院大学 | Method for producing carbon nanotube dispersion |
| WO2007007594A1 (en) * | 2005-07-11 | 2007-01-18 | National University Corporation NARA Institute of Science and Technology | Process for preparation of aqueous solution containing carbon nanotube |
| US8029758B2 (en) | 2005-12-06 | 2011-10-04 | Toyota Jidosha Kabushiki Kaisha | Process for producing single-walled carbon nanotubes with increased diameter |
| JP2010144926A (en) * | 2008-12-22 | 2010-07-01 | Korea Electronics Telecommun | Gas storage structure and gas storage device including the same |
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