JPS6058892B2 - Methods for storing or transporting hydrocarbon gases - Google Patents
Methods for storing or transporting hydrocarbon gasesInfo
- Publication number
- JPS6058892B2 JPS6058892B2 JP4325978A JP4325978A JPS6058892B2 JP S6058892 B2 JPS6058892 B2 JP S6058892B2 JP 4325978 A JP4325978 A JP 4325978A JP 4325978 A JP4325978 A JP 4325978A JP S6058892 B2 JPS6058892 B2 JP S6058892B2
- Authority
- JP
- Japan
- Prior art keywords
- storing
- pressure
- hydrate
- temperature
- methane
- 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.)
- Expired
Links
- 229930195733 hydrocarbon Natural products 0.000 title claims description 23
- 150000002430 hydrocarbons Chemical class 0.000 title claims description 23
- 239000004215 Carbon black (E152) Substances 0.000 title claims description 22
- 238000000034 method Methods 0.000 title claims description 19
- 239000007789 gas Substances 0.000 title description 26
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical group C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 48
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 14
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 claims description 12
- ZBCBWPMODOFKDW-UHFFFAOYSA-N diethanolamine Chemical compound OCCNCCO ZBCBWPMODOFKDW-UHFFFAOYSA-N 0.000 claims description 8
- KDSNLYIMUZNERS-UHFFFAOYSA-N 2-methylpropanamine Chemical compound CC(C)CN KDSNLYIMUZNERS-UHFFFAOYSA-N 0.000 description 12
- 239000003345 natural gas Substances 0.000 description 9
- 150000004677 hydrates Chemical class 0.000 description 8
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 6
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- 238000001816 cooling Methods 0.000 description 4
- WGYKZJWCGVVSQN-UHFFFAOYSA-N propylamine Chemical compound CCCN WGYKZJWCGVVSQN-UHFFFAOYSA-N 0.000 description 4
- 239000007790 solid phase Substances 0.000 description 4
- -1 aliphatic amines Chemical class 0.000 description 3
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 230000006835 compression Effects 0.000 description 3
- 238000007906 compression Methods 0.000 description 3
- 230000000694 effects Effects 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 2
- HQABUPZFAYXKJW-UHFFFAOYSA-N butan-1-amine Chemical compound CCCCN HQABUPZFAYXKJW-UHFFFAOYSA-N 0.000 description 2
- 125000004432 carbon atom Chemical group C* 0.000 description 2
- 150000001875 compounds Chemical class 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- BMFVGAAISNGQNM-UHFFFAOYSA-N isopentylamine Chemical compound CC(C)CCN BMFVGAAISNGQNM-UHFFFAOYSA-N 0.000 description 2
- 239000001301 oxygen Substances 0.000 description 2
- 229910052760 oxygen Inorganic materials 0.000 description 2
- DWKNOLCXIFYNFV-HSZRJFAPSA-N 2-[[(2r)-1-[1-[(4-chloro-3-methylphenyl)methyl]piperidin-4-yl]-5-oxopyrrolidine-2-carbonyl]amino]-n,n,6-trimethylpyridine-4-carboxamide Chemical compound CN(C)C(=O)C1=CC(C)=NC(NC(=O)[C@@H]2N(C(=O)CC2)C2CCN(CC=3C=C(C)C(Cl)=CC=3)CC2)=C1 DWKNOLCXIFYNFV-HSZRJFAPSA-N 0.000 description 1
- 150000001412 amines Chemical class 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 238000007796 conventional method Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000002349 favourable effect Effects 0.000 description 1
- NMJORVOYSJLJGU-UHFFFAOYSA-N methane clathrate Chemical compound C.C.C.C.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O.O NMJORVOYSJLJGU-UHFFFAOYSA-N 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
Landscapes
- Filling Or Discharging Of Gas Storage Vessels (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Description
【発明の詳細な説明】
本発明は、メタンまたはエタンを主成分とする炭化水素
ガスの貯蔵または輸送方法に関し、特に低エネルギーで
上記ガスを貯蔵または輸送する方法に関するものである
。DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a method for storing or transporting a hydrocarbon gas containing methane or ethane as a main component, and particularly to a method for storing or transporting the gas with low energy.
メタンまたはエタンを主成分とする炭化水素ガスの貯蔵
または輸送船による海上輸送は、現在、液化温度まで冷
却し液化ガスとして行われているが、メタンガスの場合
−１６７Ｃという極低温の条件が必要であり、そのよう
な極めて低い温度を作成保持するには甚だ高い経費を必
要とし、明らかな不利を有する。At present, hydrocarbon gases whose main components are methane or ethane are stored or transported by sea via transport ships by cooling them to the liquefaction temperature and converting them into liquefied gases. However, in the case of methane gas, extremely low temperatures of -167C are required. However, creating and maintaining such extremely low temperatures requires significant expense and has obvious disadvantages.
また特公昭４６−１００６６号公報によると上記のよう
な極めて低い温度を用いる代わりに圧縮と冷却との組合
せを用いる方法が提案されており、例えば−１１’■７
Ｃ）１５．７５に９７ｃイという条件て大気温度、大気
圧力における正規密度の約４８走の貯蔵能力があるとさ
れているが、この方法においてもＬＮＧ法と同じく極め
て低い温度が必要でありあまり有利とは言い難い。本発
明者らはメタンまたはエタンを主成分とする炭化水素ガ
スを貯蔵または輸送するにあたつて、緩和な圧縮とわす
かな冷却を組み合わせた条件で貯蔵または輸送できる方
法について鋭意実験検討を重ね、他に類例をみない本発
明を提案するに至つた。Furthermore, according to Japanese Patent Publication No. 46-10066, a method using a combination of compression and cooling instead of using extremely low temperatures as described above has been proposed, for example -11'■7
C) It is said that there is a storage capacity of about 48 times the normal density at atmospheric temperature and atmospheric pressure under the condition of 97c in 15.75, but this method also requires an extremely low temperature like the LNG method, so it is not very practical. It's hard to say it's advantageous. The inventors of the present invention have conducted intensive experimental studies on a method for storing or transporting hydrocarbon gas containing methane or ethane as its main component under conditions that combine mild compression and slight cooling. We have come to propose the present invention, which is unprecedented.
本発明方法はメタンまたはエタンを主成分とする炭化水
素ガスを貯蔵または輸送するに際し、該炭化水素ガスを
炭素数３以上の水溶性の脂肪族アミンの存在下で水に接
触させ、上記炭化水素ガスの水和物を形成させた状態で
貯蔵または輸送することを特徴としている。In the method of the present invention, when storing or transporting a hydrocarbon gas containing methane or ethane as a main component, the hydrocarbon gas is brought into contact with water in the presence of a water-soluble aliphatic amine having 3 or more carbon atoms, and the hydrocarbon gas is It is characterized by storing or transporting gas in a hydrated state.
ここで、メタンまたはエタンを主成分とするガスとはメ
タンまたはエタンのいずれかの含有量が少なくとも５０
モル％であるガスであり、例えば油井、ガス井から産出
する天然ガスなどである。Here, the term methane or ethane-based gas means that the content of either methane or ethane is at least 50%.
Gas that is mol%, such as natural gas produced from oil or gas wells.
また、水和物は包接化合物と呼ばれ、水分子が格子を形
成し、その格子の内部に炭化水素を包接した結晶であり
、その包接した炭化水素ガスによりその化学物質名も異
なり、例えはメタンを包接した場合はメタン水和物と呼
ばれる。脂肪族アミンの存在下で炭化水素ガスの水和物
を形成させるのは、脂肪族アミンが炭化水素と水との水
和物の蒸気圧を低下させる効果があるからである。In addition, hydrates are called clathrate compounds, which are crystals in which water molecules form a lattice and hydrocarbons are included inside the lattice, and the names of the chemical substances differ depending on the hydrocarbon gas included. For example, when methane is included, it is called methane hydrate. The reason why a hydrate of a hydrocarbon gas is formed in the presence of an aliphatic amine is that the aliphatic amine has the effect of lowering the vapor pressure of a hydrate of a hydrocarbon and water.
この効果については水中に脂肪族アミン・が溶解してい
ると、脂肪族アミンと炭化水素ガスとの間にはアミンの
炭化水素基が存在し水と大きな親和性をもつために水和
物を形成させる上で炭化水素分子と水分子との親和性が
大きくなることが考えられる。ここで用いられる脂肪族
アミンとしては水に溶けるものならば何でもよいが、そ
の取扱いの上からｎ−プロピルアミン、ＩｓＯ−ブチル
アミン、ＩｓＯ−ペンチルアミン等の炭素数３以上の脂
肪族アミンが用いられる。第１図に上記効果について試
験した結果の一例を示す。第１図はメタン９８．７モル
％、窒素０．４モル％、酸素０．２モル％、炭酸ガス０
．７モル％という組成の天然ガスを用いて水和物を形成
させた場合の各温度におけるその蒸気圧を示すものであ
る。実線は１Ｓ０−ブチルアミンを添加した際の水和物
の蒸気圧を、点線はＩｓＯ−ブチルアミンを添加しない
場合の水和物の蒸気圧を示す。この両者を比較すれば理
解できるようにＩｓＯ−ブチルアミンは常温における水
和物の蒸気圧を極めて低下させている。従つてＩｓＯ−
ブチルアミンの添加により、従来の水和物を形成条件よ
り遥かに低い圧力で水和物を作ることが常温においてで
きるために、ＬＮＧ法ならびにその他種々提案されてい
る方法より極めて有利な条件での貯蔵または輸送が可能
となる。本発明方法において脂肪族アミンの使用量は水
に対して０．１〜２踵量％程度で充分である。Regarding this effect, when an aliphatic amine is dissolved in water, the hydrocarbon group of the amine exists between the aliphatic amine and the hydrocarbon gas, and it has a large affinity for water, resulting in a hydrate. It is thought that the affinity between hydrocarbon molecules and water molecules increases in forming them. The aliphatic amine used here may be anything as long as it is soluble in water, but from the viewpoint of handling, aliphatic amines having 3 or more carbon atoms such as n-propylamine, IsO-butylamine, IsO-pentylamine, etc. are used. . FIG. 1 shows an example of the results of testing for the above effects. Figure 1 shows 98.7 mol% methane, 0.4 mol% nitrogen, 0.2 mol% oxygen, and 0 carbon dioxide.
．． It shows the vapor pressure at each temperature when a hydrate is formed using natural gas having a composition of 7 mol%. The solid line shows the vapor pressure of the hydrate when 1S0-butylamine is added, and the dotted line shows the vapor pressure of the hydrate when IsO-butylamine is not added. As can be understood by comparing the two, IsO-butylamine significantly lowers the vapor pressure of the hydrate at room temperature. Therefore IsO-
By adding butylamine, hydrates can be formed at room temperature at a pressure far lower than conventional hydrate formation conditions, making storage conditions extremely advantageous compared to the LNG method and various other proposed methods. Or transportation becomes possible. In the method of the present invention, the amount of aliphatic amine used is approximately 0.1 to 2% by weight based on water.
また、本発明方法において水和物を形成させる温度は５
０゜Ｃ以下とすることが望ましい。これは、水和物は低
温ほど形成されやすく、大気温度としてはかなりの高温
てある５０℃より高い温度て水和物を形成させることは
非常に不利となるからである。また、水和物を形成させ
る圧力は５０ｋ９１ｃ７１ｆＧ１）．ζ下とすることが
望ましい。Furthermore, in the method of the present invention, the temperature at which hydrates are formed is 5
It is desirable to keep the temperature below 0°C. This is because hydrates are more likely to be formed at lower temperatures, and it is very disadvantageous to form hydrates at temperatures higher than 50° C., which is quite high in terms of atmospheric temperature. Also, the pressure for forming hydrates is 50k91c71fG1). It is desirable that it be below ζ.
これは、水和物は高圧ほど形成されやすいが、５０ｋ９
１ｃＩｔＧより高い圧力で炭化水素ガスの水和物を形成
させることは、その貯蔵容器の肉厚が非常に厚いものが
必要となり従来のＬＮＧ法などと比べて有利にならない
といこう理由からである。なお、本発明方法において温
度５０℃以下、圧力５０ｋ９１ｃ１１Ｇ以下という条件
て炭化水素ガスの水和物を形成させて貯蔵または輸送し
、それから炭化水素ガスを回収するには、水和物の形成
する条件ダより高い温度または低い圧力にすれば容易に
炭化水素ガスを回収できる。This is because hydrates are more likely to be formed at higher pressures, but 50k9
This is because forming a hydrocarbon gas hydrate at a pressure higher than 1 cItG requires a very thick storage container, which is not advantageous compared to the conventional LNG method. In addition, in the method of the present invention, in order to form a hydrate of hydrocarbon gas under the conditions of a temperature of 50° C. or less and a pressure of 50 k91c11 G or less, and store or transport the hydrocarbon gas, and then recover the hydrocarbon gas, the conditions for forming the hydrate are Hydrocarbon gas can be easily recovered by raising the temperature or pressure to a higher temperature or lower pressure.
実施例１
容量２′のオートクレーブ中にＩｓＯ−ブチルアミンを
１０重量％含有した水を１．５ｅ入れ、メタンを９８．
７モル％含む天然ガスを吹き込んだところ、温度６℃、
圧力１７ｋ９１ｃＩｔＧという条件で天然ガスを０．２
３Ｎｄ貯蔵でき、また減圧により同量回収てきた。Example 1 1.5e of water containing 10% by weight of IsO-butylamine was placed in an autoclave with a capacity of 2', and 98% of methane was added.
When natural gas containing 7 mol% was blown, the temperature was 6°C,
0.2 natural gas under the condition of pressure 17k91cItG
3Nd could be stored, and the same amount could be recovered under reduced pressure.
この場合の貯蔵容量はオートクレーブ１ｅ当たりメタン
０．１１５Ｎｄであり、この値は上記条件と同じ温度、
圧力下で単に圧縮する場合の６倍程度の貯蔵能力があり
、また同じオートクレーブに−１６１℃でＬＮＧという
形態で１．５ｅ貯蔵する場合Ｊ（オートクレーブ１ｅ当
たりメタン０．４５Ｎｄ）の４分の１程度の貯蔵能力が
ある。以上のように本発明は、従来の液化法と比較して
貯蔵能力か若干低いが、液化工程が不要てあること及ひ
極めて低い温度で貯蔵する必要がないという特徴があり
、総合的に評価すると本発明は従来の液化法と比較して
非常に有利である。実施例２
容量２１のオートクレーブ中にＩｓＯ−ブチルアミンを
１０重量パーセント含有した水を１．５１入れ、メタン
９８．７モル％、窒素０．４モル％、酸素０．２モル％
、炭酸ガス０．７モル％という組成の気相状の天然ガス
を吹き込んだところ温度６℃、圧力１５．５ｋ９１ｃイ
Ｇという条件で固相の水和物が生成した。The storage capacity in this case is 0.115 Nd of methane per autoclave 1e, and this value is the same temperature as above,
The storage capacity is about 6 times that of simply compressing it under pressure, and when storing 1.5e in the form of LNG at -161℃ in the same autoclave, it has a storage capacity of 1/4 of J (0.45Nd of methane per 1e of autoclave). It has a certain storage capacity. As described above, although the storage capacity of the present invention is slightly lower than that of conventional liquefaction methods, it has the characteristics of not requiring a liquefaction process and not requiring storage at extremely low temperatures, and is therefore evaluated comprehensively. The present invention is then very advantageous compared to conventional liquefaction methods. Example 2 Into an autoclave with a capacity of 21, 1.51 mol of water containing 10% by weight of IsO-butylamine was placed, and 98.7 mol% of methane, 0.4 mol% of nitrogen, and 0.2 mol% of oxygen were added.
When gaseous natural gas having a composition of 0.7 mol % carbon dioxide was blown into the reactor, a solid phase hydrate was produced under the conditions of a temperature of 6° C. and a pressure of 15.5 k91 g.
オートクレーブ内の圧力が１６ｋ９１ｃＩｔＧで一定に
なるまでに吹き込んだ天然ガスの量は０．２１Ｎｄであ
り、またオートクレーブ内を減圧にして圧力を大気圧ま
で減少させた時に回収できた天然ガスは吹き込んだ量と
同じてあつた。実施例３
実施例２と同様の実験をｎ−プロピルアミンを１鍾量パ
ーセント含有した水を用いて行つたところ、固相の水和
物が生成する条件は温度４℃、圧力４８ｋｇ１ｃ７７ｆ
Ｇてあり、オートクレーブに吹き込んだ天然ガスの量及
び回収できた天然ガスの量については実施例１と同様の
結果が得られた。The amount of natural gas injected until the pressure inside the autoclave became constant at 16k91cItG was 0.21Nd, and the amount of natural gas that was recovered when the pressure inside the autoclave was reduced to atmospheric pressure was blown in. It was the same. Example 3 When the same experiment as in Example 2 was conducted using water containing 1 weight percent of n-propylamine, the conditions for forming a solid phase hydrate were a temperature of 4°C and a pressure of 48 kg 1c77f.
G, and the same results as in Example 1 were obtained regarding the amount of natural gas blown into the autoclave and the amount of natural gas recovered.
実施例４
容量２′のオートクレーブ中にＩｓＯ−ブチルアミンを
１０重量パーセント含有した水を１．５′入れ、エタン
９９モル％、窒素０．３モル％、炭酸ガス０．７モル％
という組成の気相状のエタンガスを吹き込んだところ、
温度６℃、圧力４ｋ９１ｄＧという条件で固相の水和物
が生成した。Example 4 1.5' of water containing 10% by weight of IsO-butylamine was placed in an autoclave with a capacity of 2', and 99 mol% of ethane, 0.3 mol% of nitrogen, and 0.7 mol% of carbon dioxide were added.
When gaseous ethane gas with the composition was blown into it,
A solid phase hydrate was produced under the conditions of a temperature of 6°C and a pressure of 4k91dG.
オートクレーブ内の圧力が４ｋ９１ｃ７１ｆＧで一定に
なるまで吹き込んだエタンガスの量は０．２５ＮＴｒＩ
であり、またオートクレーブ内を減圧にして圧力を大気
圧まて減少させた時に回収できたエタンガスは吹き込ん
だ量と同じであつた。同様の実験を何も添加しない水を
用いて行つたところ、温度６℃、圧力９ｋｇＩｃ１ｔＧ
という条件で固相の水和物が生成した。以上説明したよ
うに本発明は従来極めて低い温度まで冷却し液化ガスと
して貯蔵または輸送していたメタンまたはエタンを主成
分とする炭化水素ガスを緩和な圧縮とわずかな冷却を組
み合わせ、脂肪族アミンの存在下で水和物を形成させる
ことにより、従来法より非常に有利な条件で貯蔵または
輸送できるという利点がある。The amount of ethane gas injected until the pressure inside the autoclave became constant at 4k91c71fG was 0.25NTrI.
When the pressure inside the autoclave was reduced to atmospheric pressure, the amount of ethane gas recovered was the same as the amount blown into the autoclave. When a similar experiment was conducted using water without any addition, the temperature was 6℃ and the pressure was 9kgIc1tG.
A solid phase hydrate was formed under these conditions. As explained above, the present invention combines mild compression and slight cooling of hydrocarbon gases mainly composed of methane or ethane, which have conventionally been cooled to extremely low temperatures and stored or transported as liquefied gases, to produce aliphatic amines. The advantage of forming hydrates in the presence of such compounds is that they can be stored or transported under much more favorable conditions than conventional methods.
第１図は本発明による方法の原理を説明するための水和
物の各温度における蒸気圧を示す線図である。FIG. 1 is a diagram showing the vapor pressure of a hydrate at each temperature for explaining the principle of the method according to the present invention.
Claims (1)
貯蔵または輸送するに際し、該炭化水素ガスを炭素数３
以上の水溶性の脂肪族アミンの存在下で水に接触させ、
上記炭化水素ガスの水和物を形成させた状態で貯蔵また
は輸送することを特徴とする炭化水素ガスの貯蔵または
輸送方法。1 When storing or transporting hydrocarbon gas whose main component is methane or ethane, the hydrocarbon gas must be
Contact with water in the presence of a water-soluble aliphatic amine of
A method for storing or transporting a hydrocarbon gas, comprising storing or transporting the hydrocarbon gas in a hydrated state.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4325978A JPS6058892B2 (en) | 1978-04-14 | 1978-04-14 | Methods for storing or transporting hydrocarbon gases |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4325978A JPS6058892B2 (en) | 1978-04-14 | 1978-04-14 | Methods for storing or transporting hydrocarbon gases |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS54135708A JPS54135708A (en) | 1979-10-22 |
| JPS6058892B2 true JPS6058892B2 (en) | 1985-12-23 |
Family
ID=12658848
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP4325978A Expired JPS6058892B2 (en) | 1978-04-14 | 1978-04-14 | Methods for storing or transporting hydrocarbon gases |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6058892B2 (en) |
Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2987686B2 (en) * | 1996-01-31 | 1999-12-06 | 東京瓦斯株式会社 | Gas storage method |
| KR100264819B1 (en) * | 1997-04-25 | 2000-10-02 | 안자이 구니오 | Method for utilization of meterial comprising a hydrate-like product of gases and tank therefor |
| JPH10299997A (en) * | 1997-04-28 | 1998-11-13 | Tokyo Gas Co Ltd | BOG treatment method and apparatus for low temperature liquid storage tank |
| JP2012111734A (en) * | 2010-11-26 | 2012-06-14 | Mitsui Eng & Shipbuild Co Ltd | Method for storing ethane hydrate |
-
1978
- 1978-04-14 JP JP4325978A patent/JPS6058892B2/en not_active Expired
Also Published As
| Publication number | Publication date |
|---|---|
| JPS54135708A (en) | 1979-10-22 |
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