JP2002363114A - Apparatus for separating and recovering perfluoro compound gas - Google Patents

Apparatus for separating and recovering perfluoro compound gas

Info

Publication number
JP2002363114A
JP2002363114A JP2001165873A JP2001165873A JP2002363114A JP 2002363114 A JP2002363114 A JP 2002363114A JP 2001165873 A JP2001165873 A JP 2001165873A JP 2001165873 A JP2001165873 A JP 2001165873A JP 2002363114 A JP2002363114 A JP 2002363114A
Authority
JP
Japan
Prior art keywords
gas
membrane
separation means
membrane separation
permeated
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
Application number
JP2001165873A
Other languages
Japanese (ja)
Other versions
JP3727552B2 (en
Inventor
Akihiko Nitta
昭彦 新田
Katsuto Edasawa
克人 枝澤
Takeshi Manabe
岳史 真鍋
Kozo Oya
浩三 大矢
Shuji Nagano
修次 永野
Kenichi Hachitaka
賢一 八高
Hideki Ando
秀樹 安藤
Masatoshi Goto
正敏 後藤
Takaaki Kimura
隆章 記村
Takashi Kamimura
隆 上村
Yasushi Nakabo
康司 中坊
Akira Sekiya
章 関屋
Kenji Haratani
賢治 原谷
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
National Institute of Advanced Industrial Science and Technology AIST
Semiconductor Leading Edge Technologies Inc
Research Institute of Innovative Technology for the Earth RITE
Original Assignee
National Institute of Advanced Industrial Science and Technology AIST
Semiconductor Leading Edge Technologies Inc
Research Institute of Innovative Technology for the Earth RITE
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by National Institute of Advanced Industrial Science and Technology AIST, Semiconductor Leading Edge Technologies Inc, Research Institute of Innovative Technology for the Earth RITE filed Critical National Institute of Advanced Industrial Science and Technology AIST
Priority to JP2001165873A priority Critical patent/JP3727552B2/en
Publication of JP2002363114A publication Critical patent/JP2002363114A/en
Application granted granted Critical
Publication of JP3727552B2 publication Critical patent/JP3727552B2/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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Classifications

    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00Technologies relating to chemical industry
    • Y02P20/151Reduction of greenhouse gas [GHG] emissions, e.g. CO2
    • Y02P20/155Perfluorocarbons [PFC]; Hydrofluorocarbons [HFC]; Hydrochlorofluorocarbons [HCFC]; Chlorofluorocarbons [CFC]

Landscapes

  • Separation Using Semi-Permeable Membranes (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)

Abstract

PROBLEM TO BE SOLVED: To provide an apparatus for separating and recovering a perfluoro compound gas by which the perfluoro compound gas can more efficiently be separated and recovered. SOLUTION: This apparatus is equipped with a first to a third membrane separating means 2-4 for separating the perfluoro compound gas in a gas mixture, a permeated gas returning passage 5 for feeding the resultant permeated gases from the membrane separating means 3 and 4 to the upstream side of the first membrane separating means 2, a permeated gas membrane separating means 6 for separating the perfluoro compound gas in the permeated gas from the first membrane separating means 2 and an unpermeated gas returning passage 7 for feeding the unpermeated gas from the membrane separating means 6 to the upstream side of the first membrane separating means 2.

Description

【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION

【0001】[0001]

【発明の属する技術分野】本発明は、半導体製造などに
おいて用いられるCF4、C26、C38、C4 10、S
6、NF3などのパーフルオロ化合物ガスを分離回収す
る装置に関する。
BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention
CF used inFour, CTwoF6, CThreeF8, CFourF Ten, S
F6, NFThreeSeparation and recovery of perfluoro compound gas such as
Device.

【0002】[0002]

【従来の技術】半導体製造などにおいては、エッチン
グ、洗浄等の工程に、CF4、C26、C38、C
410、SF6、NF3などのパーフルオロ化合物ガスが
用いられている。パーフルオロ化合物ガスは、地球環境
に対し有害なガス(例えば温室効果ガス)となり得るこ
とが指摘されている。このため、半導体製造工程などか
ら排出されるガス混合物からパーフルオロ化合物ガスを
分離回収し、再利用することが行われている。パーフル
オロ化合物ガスを分離回収する装置としては、膜分離、
吸着分離、蒸留分離によりパーフルオロ化合物ガスを分
離できるものがあり、特に、分離性能に優れた膜分離を
採用した分離回収装置が多く用いられている。
2. Description of the Related Art In semiconductor manufacturing and the like, CF 4 , C 2 F 6 , C 3 F 8 , C 3
4 F 10, perfluoro compound gas such as SF 6, NF 3 is used. It has been pointed out that perfluoro compound gas can be harmful to the global environment (for example, greenhouse gas). For this reason, a perfluoro compound gas is separated and recovered from a gas mixture discharged from a semiconductor manufacturing process or the like and reused. Devices for separating and recovering perfluoro compound gas include membrane separation,
There are some which can separate a perfluoro compound gas by adsorption separation and distillation separation. In particular, a separation and recovery apparatus employing a membrane separation having excellent separation performance is often used.

【0003】[0003]

【発明が解決しようとする課題】しかしながら、上記従
来の分離回収装置では、パーフルオロ化合物ガスの回収
率が不十分となる問題があった。また分離条件などを調
節することにより回収率の向上を図ると、回収ガス中の
パーフルオロ化合物ガス濃度が低くなり、回収ガスの再
利用が容易でなくなることがあった。特に、ガス混合物
中のパーフルオロ化合物ガス濃度が低い(例えば500
mg/l以下)場合に、パーフルオロ化合物ガスの回収
率、または回収ガス中のパーフルオロ化合物ガス濃度が
低くなることがあった。本発明は、上記事情に鑑みてな
されたもので、パーフルオロ化合物ガスを効率よく分離
回収することができ、しかもパーフルオロ化合物ガス濃
度が高い回収物を得ることができる分離回収装置を提供
することを目的とする。
However, the conventional separation and recovery apparatus has a problem that the recovery rate of the perfluoro compound gas is insufficient. In addition, when the recovery rate is improved by adjusting the separation conditions and the like, the concentration of the perfluoro compound gas in the recovered gas becomes low, and it may be difficult to reuse the recovered gas. In particular, the concentration of the perfluoro compound gas in the gas mixture is low (eg, 500
mg / l or less), the recovery rate of the perfluoro compound gas or the concentration of the perfluoro compound gas in the recovered gas was sometimes reduced. The present invention has been made in view of the above circumstances, and provides a separation / recovery apparatus capable of efficiently separating and recovering a perfluoro compound gas and obtaining a recovered substance having a high perfluoro compound gas concentration. With the goal.

【0004】[0004]

【課題を解決するための手段】本発明のパーフルオロ化
合物ガスの分離回収装置は、パーフルオロ化合物ガスを
含むガス混合物中のパーフルオロ化合物ガスを非透過成
分として分離する第1膜分離手段と、この膜分離手段を
経た非透過ガス中のパーフルオロ化合物ガスを非透過成
分として分離する第2膜分離手段と、第1膜分離手段か
らの透過ガス中のパーフルオロ化合物ガスを非透過成分
として分離する透過ガス膜分離手段と、この膜分離手段
からの非透過ガスを第1膜分離手段の上流側に送る非透
過ガス返送経路とを備えていることを特徴とする。透過
ガス膜分離手段は、前記透過ガスを膜分離するにあたっ
て、この透過ガスを分離膜の外部側から内部側へ透過さ
せる外圧式構造とするのが好ましい。透過ガス膜分離手
段は、分離膜内部を減圧することによって、分離膜外部
側から内部側へのガス透過を促すことができるように構
成されていることが好ましい。透過ガス膜分離手段は、
分離膜が中空糸状に形成されていることが好ましい。本
発明の分離回収装置は、第2膜分離手段からの透過ガス
を、第1膜分離手段の上流側に送る透過ガス返送経路を
備えた構成とするのが好ましい。
According to the present invention, there is provided a perfluoro compound gas separation / recovery apparatus comprising: a first membrane separation means for separating a perfluoro compound gas in a gas mixture containing the perfluoro compound gas as a non-permeating component; A second membrane separation means for separating a perfluoro compound gas in the non-permeate gas passing through the membrane separation means as a non-permeate component, and a perfluoro compound gas in the permeate gas from the first membrane separation means as a non-permeate component And a non-permeate gas return path for sending the non-permeate gas from the membrane separator to the upstream side of the first membrane separator. It is preferable that the permeable gas membrane separation means has an external pressure structure in which the permeable gas is permeated from the outside to the inside of the separation membrane when the permeable gas is subjected to membrane separation. It is preferable that the permeable gas membrane separation means is configured to be able to promote gas permeation from the outside to the inside of the separation membrane by reducing the pressure inside the separation membrane. The permeable gas membrane separation means,
It is preferable that the separation membrane is formed in a hollow fiber shape. It is preferable that the separation and recovery apparatus of the present invention has a configuration provided with a permeated gas return path for sending the permeated gas from the second membrane separation means to the upstream side of the first membrane separation means.

【0005】[0005]

【発明の実施の形態】図1は、本発明のパーフルオロ化
合物ガス(以下、PFCガスという)の分離回収装置の
一実施形態を示すものである。図1において、符号1
は、PFCガスを含むガス混合物を昇圧させる昇圧機、
符号2は、昇圧されたガス混合物中のPFCガスを非透
過成分として分離する第1膜分離手段、符号3は、第1
膜分離手段2を経た非透過ガス中のPFCガスを非透過
成分として分離する第2膜分離手段、符号4は、第2膜
分離手段3を経た非透過ガス中のPFCガスを非透過成
分として分離する第3膜分離手段、符号5は、第2およ
び第3膜分離手段3、4からの透過ガスを第1膜分離手
段2の上流側に送る透過ガス返送経路、符号6は、第1
膜分離手段2からの透過ガス中のPFCガスを非透過成
分として分離する透過ガス膜分離手段、符号7は、透過
ガス膜分離手段6からの非透過ガスを第1膜分離手段2
の上流側に送る非透過ガス返送経路を示す。
FIG. 1 shows an embodiment of the apparatus for separating and recovering perfluoro compound gas (hereinafter referred to as PFC gas) of the present invention. In FIG.
Is a pressurizer that pressurizes a gas mixture containing PFC gas,
Reference numeral 2 denotes a first membrane separation unit for separating the PFC gas in the pressurized gas mixture as a non-permeating component, and reference numeral 3 denotes a first membrane separation unit.
A second membrane separation unit, which separates the PFC gas in the non-permeate gas that has passed through the membrane separation unit 2 as a non-permeate component, is denoted by reference numeral 4 as a PFC gas in the non-permeate gas that has passed through the second membrane separation unit 3 as a non-permeate component. Reference numeral 5 denotes a third membrane separation unit that separates the permeated gas from the second and third membrane separation units 3 and 4, and a permeated gas return path that sends the permeated gas to the upstream side of the first membrane separation unit 2.
The permeable gas membrane separation means for separating the PFC gas in the permeable gas from the membrane separation means 2 as a non-permeable component, and the reference numeral 7 designates the non-permeable gas from the permeable gas membrane separation means 6 as the first membrane separation means 2.
2 shows a non-permeate gas return path to be sent to the upstream side.

【0006】第1〜第3膜分離手段2〜4は、中空糸
状、管状、スパイラル状などの分離膜を備えた構成とす
ることができる。膜分離手段2〜4には、膜分離にあた
って、ガスを分離膜の外部側から内部側へ透過させる外
圧式構造を採用してもよいし、ガスを分離膜の内部側か
ら外部側へ透過させる内圧式構造を採用してもよい。
[0006] The first to third membrane separation means 2 to 4 can be configured to have a separation membrane in a hollow fiber shape, a tubular shape, a spiral shape or the like. The membrane separation means 2 to 4 may employ an external pressure type structure that allows gas to pass from the outside to the inside of the separation membrane during membrane separation, or allows gas to pass from the inside to the outside of the separation membrane. An internal pressure type structure may be adopted.

【0007】透過ガス膜分離手段6は、中空糸状、管
状、スパイラル状などの分離膜を備えた構成とすること
ができる。なかでも特に、中空糸状の分離膜を用いる
と、膜面積を大きくできるため好ましい。
[0007] The permeated gas membrane separation means 6 can be provided with a separation membrane of a hollow fiber shape, a tubular shape, a spiral shape or the like. In particular, it is preferable to use a hollow fiber-shaped separation membrane because the membrane area can be increased.

【0008】透過ガス膜分離手段6には、第1膜分離手
段2からの透過ガスを膜分離するにあたって、この透過
ガスを分離膜の外部側から内部側へ透過させる外圧式構
造を採用するのが好ましい。図2は、外圧式構造の透過
ガス膜分離手段6の一例を示すもので、ここに示す透過
ガス膜分離手段6は、外容器8内に中空糸状分離膜9が
設けられ、これら外容器8と分離膜9との間に導入され
た導入ガスG1の一部を分離膜9内部に透過させ、透過
ガスG2を得ることができる構造とされている。なお符
号G3は非透過ガスを示す。透過ガス膜分離手段6は、
分離膜9内部を減圧ポンプ10によって減圧することに
よって、分離膜9内外の圧力差により外部側から内部側
へのガス透過を促すことができる構成とするのが好まし
い。なお、透過ガス膜分離手段6としては、外圧式構造
に限らず、上記透過ガスを分離膜の内部側から外部側へ
透過させる内圧式構造を採用することもできる。
When the permeated gas from the first membrane separation means 2 is subjected to membrane separation, the permeated gas membrane separation means 6 employs an external pressure type structure for permeating the permeated gas from the outside to the inside of the separation membrane. Is preferred. FIG. 2 shows an example of the permeated gas membrane separation means 6 having an external pressure type structure. The permeated gas membrane separation means 6 shown here is provided with a hollow fiber-like separation membrane 9 in an outer container 8, A part of the introduced gas G1 introduced between the gas and the separation membrane 9 is transmitted through the inside of the separation membrane 9 to obtain a permeated gas G2. The symbol G3 indicates a non-permeated gas. The permeated gas membrane separation means 6
By depressurizing the inside of the separation membrane 9 with the decompression pump 10, it is preferable that the pressure difference between the inside and outside of the separation membrane 9 promotes gas permeation from the outside to the inside. The permeable gas membrane separation means 6 is not limited to the external pressure type structure, but may employ an internal pressure type structure that allows the permeated gas to permeate from the inside to the outside of the separation membrane.

【0009】膜分離手段2〜4、6に用いられる分離膜
としては、有機高分子材料(ポリスルフォン系、ポリイ
ミド系、ポリオレフィン系、セルロース系、ポリビニル
アルコール系等)からなるものを用いることができる。
また分離膜としては、上記有機高分子材料膜を、熱処理
により炭素化して得られた炭素膜を用いることもでき
る。炭素膜としては、例えば上記有機高分子材料からな
る膜を、不活性ガス(窒素等)雰囲気下において500
〜900℃で熱処理し、少なくとも一部を炭素化したも
のを用いることができる。
As the separation membrane used in the membrane separation means 2 to 4 and 6, a separation membrane made of an organic polymer material (polysulfone, polyimide, polyolefin, cellulose, polyvinyl alcohol, etc.) can be used. .
Further, as the separation membrane, a carbon membrane obtained by carbonizing the above-mentioned organic polymer material membrane by heat treatment can also be used. As the carbon film, for example, a film made of the above-mentioned organic polymer material is formed in an inert gas (nitrogen or the like) atmosphere for 500 minutes.
Heat treated at about 900 ° C. and carbonized at least in part can be used.

【0010】次に、図1に示す分離回収装置1を用いた
場合を例として、本発明の分離回収方法の一実施形態を
説明する。本実施形態の分離回収方法の対象となるガス
混合物としては、半導体製造工程などからの排出された
PFCガス含有ガスを例示できる。例えば、PFCガス
(CF4、C26、C38、C410、SF6、NF3
ど)と他成分ガス(不活性ガス、二酸化炭素、空気な
ど)とを含むものを例示できる。不活性ガスとしては窒
素、アルゴンを例示できる。
Next, an embodiment of the separation and recovery method of the present invention will be described by taking as an example the case where the separation and recovery apparatus 1 shown in FIG. 1 is used. Examples of the gas mixture to be subjected to the separation and recovery method of the present embodiment include a PFC gas-containing gas discharged from a semiconductor manufacturing process or the like. For example, a gas containing a PFC gas (CF 4 , C 2 F 6 , C 3 F 8 , C 4 F 10 , SF 6 , NF 3, etc.) and another component gas (inert gas, carbon dioxide, air, etc.) Can be illustrated. Examples of the inert gas include nitrogen and argon.

【0011】このガス混合物を、経路11を通して昇圧
機1に導入し、ここで昇圧した後、経路12を通して第
1膜分離手段2に導入する。第1膜分離手段2において
は、ガス混合物中の他成分ガス(窒素ガス等)の大部分
が分離膜を透過し、透過ガスとして経路13に導出され
る。一方、ガス混合物中のPFCガスの多くの部分は分
離膜を透過せず、PFCガスが濃縮された非透過ガス
(非透過成分)として経路14を通して第2膜分離手段
3に送られる。この際、PFCガスの多くの部分は第2
膜分離手段3に送られるものの、PFCガスの一部は、
分離膜を透過し、上記他成分ガスとともに透過ガスとし
て経路13に導出される。
The gas mixture is introduced into the pressure booster 1 through a path 11, where the pressure is increased. Then, the gas mixture is introduced into the first membrane separation means 2 through a path 12. In the first membrane separation means 2, most of the other component gas (such as nitrogen gas) in the gas mixture permeates the separation membrane and is led out to the passage 13 as a permeated gas. On the other hand, most of the PFC gas in the gas mixture does not pass through the separation membrane, and is sent to the second membrane separation means 3 through the passage 14 as a non-permeate gas (non-permeate component) in which the PFC gas is concentrated. At this time, most of the PFC gas is
Although sent to the membrane separation means 3, part of the PFC gas is
After passing through the separation membrane, it is led to the passage 13 as a permeated gas together with the other component gas.

【0012】第2膜分離手段3では、経路14からの非
透過ガス中のPFCガスがさらに濃縮され、非透過ガス
(非透過成分)として経路15を通して第3膜分離手段
4に送られる。第2膜分離手段3の透過ガスは、透過ガ
ス返送経路5によって、経路11を経て再び昇圧機1に
導入される。これによって透過ガス中の残留PFCガス
は再び膜分離手段2〜4に供給される。
In the second membrane separation means 3, the PFC gas in the non-permeate gas from the passage 14 is further concentrated and sent to the third membrane separation means 4 through the passage 15 as a non-permeate gas (non-permeate component). The permeated gas of the second membrane separation means 3 is again introduced into the booster 1 through the permeated gas return path 5 via the path 11. Thereby, the residual PFC gas in the permeated gas is supplied again to the membrane separation means 2 to 4.

【0013】第3膜分離手段4では、経路15からの非
透過ガス中のPFCガスがさらに濃縮され、非透過ガス
(非透過成分)として経路16を通して回収される(以
下、分離回収ガスという)。第3膜分離手段4の透過ガ
スは、透過ガス返送経路5によって、経路11を経て再
び昇圧機1に導入される。これによって透過ガス中の残
留PFCガスは再び膜分離手段2〜4に供給される。
In the third membrane separation means 4, the PFC gas in the non-permeate gas from the passage 15 is further concentrated and recovered as a non-permeate gas (non-permeate component) through the passage 16 (hereinafter, referred to as a separated and recovered gas). . The permeated gas of the third membrane separation means 4 is again introduced into the booster 1 through the permeated gas return path 5 via the path 11. Thereby, the residual PFC gas in the permeated gas is supplied again to the membrane separation means 2 to 4.

【0014】上述のように、第1膜分離手段2におい
て、ガス混合物中のPFCガスの一部は、分離膜を透過
し、上記他成分ガスとともに透過ガスとして経路13に
導出される。この透過ガスは、経路13を通して導入ガ
スG1として透過ガス膜分離手段6に導入される。
As described above, in the first membrane separation means 2, a part of the PFC gas in the gas mixture permeates the separation membrane and is led out to the passage 13 as a permeated gas together with the other component gases. This permeated gas is introduced into the permeated gas membrane separation means 6 through the passage 13 as the introduced gas G1.

【0015】図2に示すように、透過ガス膜分離手段6
では、減圧ポンプ10によって分離膜9内部を減圧す
る。これによって、導入ガスG1中の他成分ガスは、分
離膜9内外の圧力差により透過ガスG2として経路17
を通して系外に導出される。導入ガスG1中のPFCガ
スは、非透過ガス返送経路7を通して非透過ガスG3
(非透過成分)として導出され、経路11を経て再び昇
圧機1に導入され、再び膜分離手段2〜4に供給され
る。
As shown in FIG. 2, the permeable gas membrane separation means 6
Then, the pressure inside the separation membrane 9 is reduced by the vacuum pump 10. As a result, the other component gas in the introduced gas G1 is converted into the permeated gas G2 by the pressure difference between the inside and outside of the separation membrane 9 as the path 17
Through the system. The PFC gas in the introduction gas G1 passes through the non-permeate gas return path 7 to pass through the non-permeate gas G3.
It is derived as a (non-permeated component), introduced again into the booster 1 via the path 11, and supplied again to the membrane separation means 2 to 4.

【0016】本実施形態の分離回収装置では、第1膜分
離手段2からの透過ガス中のPFCガスを分離する透過
ガス膜分離手段6と、透過ガス膜分離手段6からの非透
過ガスを第1膜分離手段2の上流側に送る非透過ガス返
送経路7とを備えているので、第1膜分離手段2を透過
したPFCガスを、透過ガス膜分離手段6によって回収
し、再び膜分離手段2〜4に供給することができる。こ
のため、ガス混合物中のPFCガス濃度が低い場合で
も、PFCガスの回収率を高めることができる。また透
過ガス膜分離手段6において、PFCガスを、それ以外
のガス(不活性ガスなど)から分離することができるた
め、ガス混合物中のPFCガス濃度が低い場合でも、分
離回収ガス中のPFCガス濃度を高めることができる。
このため、分離回収ガスの再利用が容易となる。
In the separation and recovery apparatus of the present embodiment, the permeated gas separation means 6 for separating the PFC gas in the permeated gas from the first membrane separation means 2 and the non-permeated gas from the permeated gas separation means 6 Since it has the non-permeate gas return path 7 for sending upstream to the first membrane separation means 2, the PFC gas permeated through the first membrane separation means 2 is collected by the permeated gas membrane separation means 6, and the membrane separation means is returned again. 2 to 4 can be supplied. For this reason, even when the PFC gas concentration in the gas mixture is low, the recovery rate of the PFC gas can be increased. Further, since the PFC gas can be separated from other gases (inert gas, etc.) in the permeated gas membrane separation means 6, even if the PFC gas concentration in the gas mixture is low, the PFC gas in the separated and collected gas can be separated. The concentration can be increased.
For this reason, it is easy to reuse the separated and collected gas.

【0017】また一般に、複数の膜分離手段を直列に配
列した分離回収装置では、供給するガスに高い圧力をか
けて分離膜内外の圧力差を大きくすることで、ガスを分
離膜の内側から外側に透過させ、非透過ガス中のPFC
ガスを高圧条件で濃縮する。この供給ガスと透過ガスと
の圧力差が大きいほど高いガス透過量が得られる。本実
施形態では、透過ガス膜分離手段6として、外圧式構造
のものを用いることによって、透過ガス膜分離手段6に
おける圧力損失を小さくすることができるため、分離膜
9内部を減圧することにより膜分離を行うことが容易と
なる。このため、導入ガスG1の圧力を高めることな
く、透過ガス膜分離手段6において良好な膜分離が可能
となる。従って、第1膜分離手段2における膜分離に悪
影響が及ぶのを防ぎ、第1膜分離手段2において高効率
でPFCガスの分離を行うことができる。これに対し、
透過ガス膜分離手段6に内圧式構造のものを用いる場合
には、圧力損失が大きくなりやすいため、効率よく膜分
離を行うには、導入ガスG1の圧力を高めることが必要
となる。このため、第1膜分離手段2においてPFCガ
スの分離効率が低下しやすくなる。これは、上述のよう
な分離に必要な、第1膜分離手段2における分離膜内外
の十分な圧力差を設定するのが難しくなるためである。
In general, in a separation and recovery apparatus in which a plurality of membrane separation means are arranged in series, a high pressure is applied to a supplied gas to increase a pressure difference between the inside and outside of the separation membrane, so that the gas is moved from inside to outside of the separation membrane. PFC in non-permeated gas
The gas is concentrated under high pressure conditions. The larger the pressure difference between the supply gas and the permeated gas, the higher the gas permeation amount can be obtained. In this embodiment, since the pressure loss in the permeated gas membrane separation means 6 can be reduced by using an external pressure type structure as the permeated gas membrane separation means 6, the pressure in the separation membrane 9 is reduced by reducing the pressure inside the separation membrane 9. Separation becomes easy. Therefore, good membrane separation can be performed in the permeated gas membrane separation means 6 without increasing the pressure of the introduced gas G1. Therefore, it is possible to prevent an adverse effect on the membrane separation in the first membrane separation unit 2 and to separate the PFC gas with high efficiency in the first membrane separation unit 2. In contrast,
When an internal pressure type structure is used for the permeable gas membrane separation means 6, the pressure loss is likely to increase. Therefore, it is necessary to increase the pressure of the introduced gas G1 in order to efficiently perform the membrane separation. For this reason, the separation efficiency of the PFC gas in the first membrane separation means 2 tends to decrease. This is because it becomes difficult to set a sufficient pressure difference between the inside and outside of the separation membrane in the first membrane separation means 2 necessary for the above-described separation.

【0018】[0018]

【実施例】以下、具体例を示して本発明の分離回収方法
を説明する。 (実施例)図1および図2に示す分離回収装置を用いて
以下の分離回収試験を行った。膜分離手段2〜4として
は内圧式構造のものを用い、透過ガス膜分離手段6とし
ては外圧式構造のものを用いた。本実施形態では、ガス
混合物として窒素とCF4の混合物を使用した。ガス混
合物中のCF4濃度は500mg/lとした。ガス混合
物の供給流量は30L/minとした。このガス混合物
を、昇圧機1で0.99MPaまで昇圧した後、第1膜
分離手段2に導入し、非透過ガスを第2膜分離手段3に
導入し、第2膜分離手段3からの非透過ガスを第3膜分
離手段4に導入し、第3膜分離手段4からの非透過ガス
を経路16を通して回収した(分離回収ガス)。膜分離
手段3、4からの透過ガスは、透過ガス返送経路5を通
して昇圧機1に返送した。膜分離手段2〜4における膜
分離時の温度条件は60℃とした。第1膜分離手段2か
ら透過ガス(導入ガスG1)を透過ガス膜分離手段6に
導入し、透過ガスG2を経路17を通して系外に排出
し、非透過ガスG3を非透過ガス返送経路7を通して昇
圧機1に返送した。膜分離手段2〜4における圧力条件
を変化させた時の分離回収ガスのCF4濃度と回収率と
の関係を図3に示す。
Hereinafter, the separation and recovery method of the present invention will be described with reference to specific examples. (Example) The following separation and recovery test was performed using the separation and recovery apparatus shown in FIGS. The internal pressure type structure was used as the membrane separation means 2 to 4, and the external pressure type structure was used as the permeated gas membrane separation means 6. In the present embodiment, a mixture of nitrogen and CF 4 was used as the gas mixture. The CF 4 concentration in the gas mixture was 500 mg / l. The supply flow rate of the gas mixture was 30 L / min. After this gas mixture is pressurized to 0.99 MPa by the pressure booster 1, it is introduced into the first membrane separation means 2, the non-permeate gas is introduced into the second membrane separation means 3, and the non-permeate gas is supplied from the second membrane separation means 3. The permeated gas was introduced into the third membrane separation means 4, and the non-permeated gas from the third membrane separation means 4 was recovered through the path 16 (separated and recovered gas). The permeated gas from the membrane separation means 3 and 4 was returned to the booster 1 through the permeated gas return path 5. The temperature condition at the time of membrane separation in the membrane separation means 2 to 4 was 60 ° C. The permeated gas (introduced gas G1) is introduced from the first membrane separation means 2 to the permeated gas membrane separation means 6, the permeated gas G2 is discharged out of the system through the path 17, and the non-permeated gas G3 is passed through the non-permeated gas return path 7. It was returned to the booster 1. FIG. 3 shows the relationship between the CF 4 concentration of the separated and recovered gas and the recovery rate when the pressure conditions in the membrane separation means 2 to 4 are changed.

【0019】(比較例)図4に示すように、透過ガス膜
分離手段6と非透過ガス返送経路7とを備えていないこ
と以外は図1に示す装置と同様の構成の分離回収装置を
用いて実施例と同様の分離回収試験を行った。この試験
では、第1膜分離手段2から透過ガスを経路13を通し
てそのまま系外に排出した。膜分離手段2〜4における
圧力条件を変化させた時の分離回収ガスのCF4濃度と
回収率との関係を図5に示す。
(Comparative Example) As shown in FIG. 4, a separation / recovery apparatus having the same configuration as the apparatus shown in FIG. 1 is used except that the permeated gas membrane separation means 6 and the non-permeated gas return path 7 are not provided. The same separation and recovery test as in the example was performed. In this test, the permeated gas was directly discharged from the first membrane separation means 2 to the outside of the system through the passage 13. FIG. 5 shows the relationship between the CF 4 concentration of the separated and recovered gas and the recovery rate when the pressure conditions in the membrane separation means 2 to 4 were changed.

【0020】図3に示すように、透過ガス膜分離手段6
を設けない比較例では、分離回収ガスのCF4濃度を高
くするとCF4回収率が低くなり、CF4回収率を高くす
ると分離回収ガス中のCF4濃度が低くなったことがわ
かる。これに対し、実施例では、高濃度のCF4を高効
率で回収することができたことがわかる。
As shown in FIG. 3, the permeable gas membrane separation means 6
With the comparative example not provided, the higher the CF 4 concentration in the separation and recovery gas CF 4 recovery rate is low, it can be seen that became low CF 4 concentration separation and recovery gas and to increase the CF 4 recovery rate. In contrast, in the examples, it can be seen that high-concentration CF 4 could be recovered with high efficiency.

【0021】[0021]

【発明の効果】以上説明したように、本発明の分離回収
装置では、第1膜分離手段からの透過ガス中のパーフル
オロ化合物ガスを分離する透過ガス膜分離手段と、この
膜分離手段からの非透過ガスを第1膜分離手段の上流側
に送る非透過ガス返送経路とを備えているので、第1膜
分離手段を透過したパーフルオロ化合物ガスを、透過ガ
ス膜分離手段によって回収し、再び第1および第2膜分
離手段に供給することができる。このため、パーフルオ
ロ化合物ガスの回収率を高めることができる。また透過
ガス膜分離手段において、パーフルオロ化合物ガスを、
それ以外のガスから分離することができるため、回収ガ
ス中のパーフルオロ化合物ガス濃度を高めることができ
る。このため、回収ガスの再利用が容易となる。
As described above, in the separation and recovery apparatus of the present invention, the permeated gas membrane separation means for separating the perfluoro compound gas in the permeated gas from the first membrane separation means, Since there is provided a non-permeate gas return path for sending the non-permeate gas to the upstream side of the first membrane separation means, the perfluoro compound gas that has passed through the first membrane separation means is collected by the permeate gas membrane separation means, and It can be supplied to the first and second membrane separation means. For this reason, the recovery rate of the perfluoro compound gas can be increased. In the permeated gas membrane separation means, the perfluoro compound gas is
Since the gas can be separated from other gases, the concentration of the perfluoro compound gas in the recovered gas can be increased. For this reason, it is easy to reuse the collected gas.

【図面の簡単な説明】[Brief description of the drawings]

【図1】 本発明のパーフルオロ化合物ガスの分離回収
装置の一実施形態を示す構成図である。
FIG. 1 is a configuration diagram showing an embodiment of a perfluoro compound gas separation / recovery device of the present invention.

【図2】 図1に示す分離回収装置の透過ガス膜分離手
段の構造図である。
FIG. 2 is a structural view of a permeated gas membrane separation means of the separation and recovery apparatus shown in FIG.

【図3】 試験結果を示すグラフである。FIG. 3 is a graph showing test results.

【図4】 分離回収装置の一例を示す構成図である。FIG. 4 is a configuration diagram illustrating an example of a separation and recovery device.

【図5】 試験結果を示すグラフである。FIG. 5 is a graph showing test results.

【符号の説明】[Explanation of symbols]

1・・・分離回収装置、2・・・第1膜分離手段、3・・・第2
膜分離手段、5・・・透過ガス返送経路、6・・・透過ガス膜
分離手段、7・・・非透過ガス返送経路、9・・・分離膜
DESCRIPTION OF SYMBOLS 1 ... Separation and collection apparatus, 2 ... 1st membrane separation means, 3 ... 2nd
Membrane separation means, 5: Permeated gas return path, 6: Permeated gas membrane separation means, 7: Non-permeated gas return path, 9: Separation membrane

───────────────────────────────────────────────────── フロントページの続き (72)発明者 新田 昭彦 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 枝澤 克人 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 真鍋 岳史 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 大矢 浩三 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 永野 修次 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 八高 賢一 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 安藤 秀樹 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 後藤 正敏 東京都港区西新橋1丁目5番13号 第8東 洋海事ビル8階 PFC回収・再利用プロ ジェクト室内 (72)発明者 記村 隆章 神奈川県横浜市戸塚区吉田町292 株式会 社半導体先端テクノロジーズPFCグルー プ内 (72)発明者 上村 隆 神奈川県横浜市戸塚区吉田町292 株式会 社半導体先端テクノロジーズPFCグルー プ内 (72)発明者 中坊 康司 神奈川県横浜市戸塚区吉田町292 株式会 社半導体先端テクノロジーズPFCグルー プ内 (72)発明者 関屋 章 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 (72)発明者 原谷 賢治 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) 4D006 GA41 HA01 HA18 HA19 HA21 HA61 JA52A JA58A KA12 KA52 KA53 KA56 KA68 MA01 MA02 MA03 MC05 MC11 MC22 MC33 MC58 MC62 NA50 PA03 PB19 PB70 PC01 4H006 AA02 AD19 BD82 BD84 EA02 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Akihiko Nitta 8th floor of the 8th Toyo Kaiji Building, 1-5-13 Nishishinbashi, Minato-ku, Tokyo PFC collection and reuse project room (72) Inventor Ezawa Katsuto 1-5-13 Nishi-Shimbashi, Minato-ku, Tokyo The 8th floor of the 8th Oriental Maritime Building PFC collection and reuse project room (72) Inventor Takefumi Manabe 1-5-13-1 Nishi-Shimbashi, Minato-ku, Tokyo (72) Inventor Kozo Oya 1-5-13 Nishi-Shimbashi, Minato-ku, Tokyo 8th Toyo Maritime Building 8th Floor PFC Collection / Reuse Room (72) Inventor Shuji Nagano 1-5-13 Nishi-Shimbashi, Minato-ku, Tokyo 8th Toyo Maritime Building 8F PFC Collection / Reuse Project Room (72) Inventor 8 Kenichi 1-5-13 Nishi-Shimbashi, Minato-ku, Tokyo Eighth Toyo Maritime Building 8F PFC Collection / Reuse Project Room (72) Inventor Hideki Ando 1-5-13-1, Nishi-Shimbashi, Minato-ku, Tokyo (72) Inventor Masatoshi Goto 1st-13-13 Nishishinbashi, Minato-ku, Tokyo 8th Oriental Maritime Building 8th Floor PFC Collection / Reuse Project Room (72) 72) Inventor Takaaki Kikimura 292, Yoshida-cho, Totsuka-ku, Yokohama-shi, Kanagawa Prefecture Inside the Semiconductor Advanced Technologies PFC Group (72) Inventor Takashi Uemura 292, Yoshida-cho, Totsuka-ku, Yokohama-shi, Kanagawa Prefecture Semiconductor Advanced Technologies PFC Group Inside (72) Inventor Yasushi Nakabo 292 Yoshida-cho, Totsuka-ku, Yokohama-shi, Kanagawa Prefecture Within the Semiconductor Advanced Technologies PFC Group (72) Inventor Akira Sekiya 1-1-1 Higashi, Tsukuba-shi, Ibaraki Independent Administrative Law Human Industrial Technology Comprehensive research Inside the Tsukuba Center (72) Inventor Kenji Haratani 1-1-1 Higashi, Tsukuba City, Ibaraki Prefecture Independent Administrative Law National Institute of Advanced Industrial Science and Technology Tsukuba Center F-term (reference) MA01 MA02 MA03 MC05 MC11 MC22 MC33 MC58 MC62 NA50 PA03 PB19 PB70 PC01 4H006 AA02 AD19 BD82 BD84 EA02

Claims (5)

【特許請求の範囲】[Claims] 【請求項1】 パーフルオロ化合物ガスを含むガス混合
物中のパーフルオロ化合物ガスを非透過成分として分離
する第1膜分離手段と、 この膜分離手段を経た非透過ガス中のパーフルオロ化合
物ガスを非透過成分として分離する第2膜分離手段と、 第1膜分離手段からの透過ガス中のパーフルオロ化合物
ガスを非透過成分として分離する透過ガス膜分離手段
と、 この膜分離手段からの非透過ガスを第1膜分離手段の上
流側に送る非透過ガス返送経路とを備えていることを特
徴とするパーフルオロ化合物ガスの分離回収装置。
1. A first membrane separation means for separating a perfluoro compound gas in a gas mixture containing a perfluoro compound gas as a non-permeate component, and a non-permeate gas in the non-permeate gas passed through the membrane separation means. A second membrane separation means for separating as a permeate component, a permeate gas separation means for separating a perfluoro compound gas in a permeate gas from the first membrane separation means as a non-permeate component, and a non-permeate gas from the membrane separation means And a non-permeate gas return path for sending the gas to the upstream side of the first membrane separation means.
【請求項2】 透過ガス膜分離手段は、前記透過ガスを
膜分離するにあたって、この透過ガスを分離膜の外部側
から内部側へ透過させる外圧式構造とされていることを
特徴とする請求項1記載のパーフルオロ化合物ガスの分
離回収装置。
2. The permeable gas membrane separation means has an external pressure type structure for permeating the permeable gas from the outside to the inside of the separation membrane when separating the permeable gas into a membrane. 2. The apparatus for separating and recovering a perfluoro compound gas according to claim 1.
【請求項3】 透過ガス膜分離手段は、分離膜内部を減
圧することによって、分離膜外部側から内部側へのガス
透過を促すことができるように構成されていることを特
徴とする請求項2記載のパーフルオロ化合物ガスの分離
回収装置。
3. The permeable gas membrane separation means is configured to be able to promote gas permeation from the outside to the inside of the separation membrane by reducing the pressure inside the separation membrane. 3. The apparatus for separating and recovering a perfluoro compound gas according to 2.
【請求項4】 透過ガス膜分離手段は、分離膜が中空糸
状に形成されていることを特徴とする請求項1〜3のう
ちいずれか1項記載のパーフルオロ化合物ガスの分離回
収装置。
4. The perfluoro compound gas separation and recovery apparatus according to claim 1, wherein the permeated gas membrane separation means has a separation membrane formed in a hollow fiber shape.
【請求項5】 第2膜分離手段からの透過ガスを、第1
膜分離手段の上流側に送る透過ガス返送経路を備えてい
ることを特徴とする請求項1〜4のうちいずれか1項記
載のパーフルオロ化合物ガスの分離回収装置。
5. The method according to claim 1, wherein the permeated gas from the second membrane separation means is supplied to the first membrane separation means.
The perfluoro compound gas separation / recovery apparatus according to any one of claims 1 to 4, further comprising a permeated gas return path for sending the gas to an upstream side of the membrane separation means.
JP2001165873A 2001-05-31 2001-05-31 Perfluoro compound gas separation and recovery equipment Expired - Lifetime JP3727552B2 (en)

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Applications Claiming Priority (1)

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Publication Number Publication Date
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JP3727552B2 JP3727552B2 (en) 2005-12-14

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2007055934A (en) * 2005-08-24 2007-03-08 Showa Denko Kk Method for production of pentafluoroethane
JP2015505273A (en) * 2011-12-27 2015-02-19 エボニック ファイバース ゲゼルシャフト ミット ベシュレンクテル ハフツングEvonik Fibres GmbH Gas separation method
JP2015525134A (en) * 2013-06-25 2015-09-03 ファインテック.カンパニー,リミテッド Perfluoro compound separation and recycling system
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