JP6062945B2 - 気体分離および液体分離用のpbi中空繊維非対称膜を製作するプロセス - Google Patents
気体分離および液体分離用のpbi中空繊維非対称膜を製作するプロセス Download PDFInfo
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- JP6062945B2 JP6062945B2 JP2014528706A JP2014528706A JP6062945B2 JP 6062945 B2 JP6062945 B2 JP 6062945B2 JP 2014528706 A JP2014528706 A JP 2014528706A JP 2014528706 A JP2014528706 A JP 2014528706A JP 6062945 B2 JP6062945 B2 JP 6062945B2
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- 239000012510 hollow fiber Substances 0.000 title claims description 52
- 238000000034 method Methods 0.000 title claims description 40
- 239000012528 membrane Substances 0.000 title claims description 25
- 239000007788 liquid Substances 0.000 title claims description 6
- 238000000926 separation method Methods 0.000 title description 6
- 230000008569 process Effects 0.000 title description 4
- 239000004693 Polybenzimidazole Substances 0.000 claims description 60
- 229920002480 polybenzimidazole Polymers 0.000 claims description 60
- 239000002904 solvent Substances 0.000 claims description 56
- 239000000243 solution Substances 0.000 claims description 53
- 229920000642 polymer Polymers 0.000 claims description 47
- 239000000835 fiber Substances 0.000 claims description 28
- 239000011148 porous material Substances 0.000 claims description 21
- 239000000463 material Substances 0.000 claims description 20
- 238000005553 drilling Methods 0.000 claims description 19
- 239000000203 mixture Substances 0.000 claims description 19
- 238000009987 spinning Methods 0.000 claims description 8
- 239000000126 substance Substances 0.000 claims description 8
- 238000010791 quenching Methods 0.000 claims description 7
- 230000000171 quenching effect Effects 0.000 claims description 7
- 239000007864 aqueous solution Substances 0.000 claims description 6
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 6
- 238000002144 chemical decomposition reaction Methods 0.000 claims description 4
- 238000005406 washing Methods 0.000 claims description 4
- 238000004804 winding Methods 0.000 claims description 4
- 239000012535 impurity Substances 0.000 claims description 3
- 238000000710 polymer precipitation Methods 0.000 claims description 3
- 239000012530 fluid Substances 0.000 description 17
- 239000007789 gas Substances 0.000 description 11
- 230000035699 permeability Effects 0.000 description 9
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- FXHOOIRPVKKKFG-UHFFFAOYSA-N N,N-Dimethylacetamide Chemical compound CN(C)C(C)=O FXHOOIRPVKKKFG-UHFFFAOYSA-N 0.000 description 6
- 208000012886 Vertigo Diseases 0.000 description 6
- 230000015572 biosynthetic process Effects 0.000 description 6
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 5
- 230000007704 transition Effects 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 4
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 4
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 4
- KWGKDLIKAYFUFQ-UHFFFAOYSA-M lithium chloride Chemical compound [Li+].[Cl-] KWGKDLIKAYFUFQ-UHFFFAOYSA-M 0.000 description 4
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 description 3
- 230000015556 catabolic process Effects 0.000 description 3
- 238000005345 coagulation Methods 0.000 description 3
- 230000015271 coagulation Effects 0.000 description 3
- 230000007423 decrease Effects 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- JUJWROOIHBZHMG-UHFFFAOYSA-N Pyridine Chemical compound C1=CC=NC=C1 JUJWROOIHBZHMG-UHFFFAOYSA-N 0.000 description 2
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 description 2
- 238000001704 evaporation Methods 0.000 description 2
- 230000008020 evaporation Effects 0.000 description 2
- 239000002657 fibrous material Substances 0.000 description 2
- 230000005484 gravity Effects 0.000 description 2
- 230000007246 mechanism Effects 0.000 description 2
- 229910052757 nitrogen Inorganic materials 0.000 description 2
- 230000035515 penetration Effects 0.000 description 2
- 229920005862 polyol Polymers 0.000 description 2
- 150000003077 polyols Chemical class 0.000 description 2
- BDERNNFJNOPAEC-UHFFFAOYSA-N propan-1-ol Chemical compound CCCO BDERNNFJNOPAEC-UHFFFAOYSA-N 0.000 description 2
- 238000007711 solidification Methods 0.000 description 2
- 230000008023 solidification Effects 0.000 description 2
- HYZJCKYKOHLVJF-UHFFFAOYSA-N 1H-benzimidazole Chemical compound C1=CC=C2NC=NC2=C1 HYZJCKYKOHLVJF-UHFFFAOYSA-N 0.000 description 1
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- 239000004372 Polyvinyl alcohol Substances 0.000 description 1
- 239000000654 additive Substances 0.000 description 1
- 150000001298 alcohols Chemical class 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 150000001720 carbohydrates Chemical class 0.000 description 1
- PBAYDYUZOSNJGU-UHFFFAOYSA-N chelidonic acid Natural products OC(=O)C1=CC(=O)C=C(C(O)=O)O1 PBAYDYUZOSNJGU-UHFFFAOYSA-N 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000010612 desalination reaction Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 235000012489 doughnuts Nutrition 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 238000012681 fiber drawing Methods 0.000 description 1
- 230000004907 flux Effects 0.000 description 1
- 150000004676 glycans Chemical class 0.000 description 1
- 150000002334 glycols Chemical group 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 125000002883 imidazolyl group Chemical group 0.000 description 1
- 239000004615 ingredient Substances 0.000 description 1
- 230000001788 irregular Effects 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000003002 pH adjusting agent Substances 0.000 description 1
- 239000002861 polymer material Substances 0.000 description 1
- 229920005597 polymer membrane Polymers 0.000 description 1
- 229920001282 polysaccharide Polymers 0.000 description 1
- 239000005017 polysaccharide Substances 0.000 description 1
- 229920002451 polyvinyl alcohol Polymers 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- UMJSCPRVCHMLSP-UHFFFAOYSA-N pyridine Natural products COC1=CC=CN=C1 UMJSCPRVCHMLSP-UHFFFAOYSA-N 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000011877 solvent mixture Substances 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 238000006277 sulfonation reaction Methods 0.000 description 1
- 230000008961 swelling Effects 0.000 description 1
- RWRDLPDLKQPQOW-UHFFFAOYSA-N tetrahydropyrrole Substances C1CCNC1 RWRDLPDLKQPQOW-UHFFFAOYSA-N 0.000 description 1
- 238000002834 transmittance Methods 0.000 description 1
- 239000004034 viscosity adjusting agent Substances 0.000 description 1
Classifications
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/12—Composite membranes; Ultra-thin membranes
- B01D69/1216—Three or more layers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/08—Hollow fibre membranes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
- B01D53/228—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion characterised by specific membranes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/02—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor characterised by their properties
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/08—Hollow fibre membranes
- B01D69/085—Details relating to the spinneret
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/08—Hollow fibre membranes
- B01D69/087—Details relating to the spinning process
- B01D69/088—Co-extrusion; Co-spinning
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/12—Composite membranes; Ultra-thin membranes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/12—Composite membranes; Ultra-thin membranes
- B01D69/1218—Layers having the same chemical composition, but different properties, e.g. pore size, molecular weight or porosity
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
- B01D71/06—Organic material
- B01D71/58—Other polymers having nitrogen in the main chain, with or without oxygen or carbon only
- B01D71/62—Polycondensates having nitrogen-containing heterocyclic rings in the main chain
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
- B01D71/06—Organic material
- B01D71/76—Macromolecular material not specifically provided for in a single one of groups B01D71/08 - B01D71/74
- B01D71/82—Macromolecular material not specifically provided for in a single one of groups B01D71/08 - B01D71/74 characterised by the presence of specified groups, e.g. introduced by chemical after-treatment
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2325/00—Details relating to properties of membranes
- B01D2325/02—Details relating to pores or porosity of the membranes
- B01D2325/022—Asymmetric membranes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2325/00—Details relating to properties of membranes
- B01D2325/02—Details relating to pores or porosity of the membranes
- B01D2325/022—Asymmetric membranes
- B01D2325/0231—Dense layers being placed on the outer side of the cross-section
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2325/00—Details relating to properties of membranes
- B01D2325/04—Characteristic thickness
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2325/00—Details relating to properties of membranes
- B01D2325/30—Chemical resistance
Landscapes
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Analytical Chemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- Separation Using Semi-Permeable Membranes (AREA)
- Artificial Filaments (AREA)
- Spinning Methods And Devices For Manufacturing Artificial Fibers (AREA)
Description
本出願は、2011年9月06日に出願された米国特許仮出願第61/531,448号の優先権を主張し、その開示は参照によってその全体が本明細書に組み込まれる。
本発明は、海軍研究事務所によって授与されたN00014−10−C−0059、およびエネルギー省によって授与されたDE−FC26−07NT43090の下に米国政府支援を受けて行われた。米国政府は本発明における一定の権利を有する。
本方法は、1〜100メートル/分の速度で繊維を繊維束に巻き取る工程をさらに含む。繊維束は、本明細書に記載されるものなどの適切な膜用途において中空繊維膜として使用することができる。
ポリベンズイミダゾールはスルホン化ポリベンズイミダゾールである。
本膜は、膜にガス混合物を通す工程を含む、H2、CO2、COおよびメタンを含むガス混合物からH2を分離する方法において使用される。
Claims (14)
- 非対称中空繊維を調製する方法であって、
(a)(i)15〜25重量%のポリベンズイミダゾール(ii)1〜5重量%のポリマーの細孔形成材料および(iii)前記ポリベンズイミダゾールについての溶媒を含むポリマー溶液をチューブインオリフィス紡糸口金の外側環状オリフィスに通す工程と、
(b)(i)前記ポリベンズイミダゾールについての65〜99重量%の非溶媒および
(ii)前記ポリベンズイミダゾールについての1〜35重量%の溶媒を含み、環形状に前記ポリマー溶液を維持する穿孔液を紡糸口金の内側チューブに通す工程と、
(c)大気中に0.3〜20cmの落下距離を有するギャップを通して、前記ポリマー溶液および前記穿孔液を落下させる工程と、
(d)浴中で前記ポリマー溶液および前記穿孔液をクエンチして、環形状を有し、第1および第2の同心層を含む非対称中空繊維を形成する工程とを含み、ここで、前記第1の層は前記第2の層と接し、多孔性でなく、前記第2の層は5〜250nmの範囲の細孔を有する多孔性であって、
前記第1の層の化学組成と前記第2の層の化学組成が同じである、該方法。 - (a)1〜100メートル/分の速度で前記繊維を繊維束に巻き取って中空繊維膜を形成する工程を含み
(b)ここで、前記ポリマー溶液は15〜25℃の温度範囲内で少なくとも6か月間化学分解に対して安定であり
(c)紡糸後の前記繊維の洗浄および延伸を含み
(d)ここで、前記ポリベンズイミダゾールはスルホン化ポリベンズイミダゾールであり、または
(e)(a)、(b)、(c)および(d)の任意の組み合わせを含む、請求項1に記載の方法。 - 前記第1の層が前記非対称中空繊維の外表面を形成し、前記第2の層は前記非対称中空繊維の内表面を形成する、請求項1に記載の方法。
- 前記第1の層が前記非対称中空繊維の内表面を形成し、前記第2の層は前記非対称中空繊維の外表面を形成する、請求項1に記載の方法。
- 前記第1の層が範囲0.1〜10μmの厚さを有し、前記第2の層は10〜500μmの範囲の厚さを有する、請求項1に記載の方法。
- 前記チューブインオリフィス紡糸口金の前記外側環状オリフィスが範囲100〜2000μmの外径を有する、請求項1に記載の方法。
- 前記第1および前記第2の層の厚さが、落下距離の長さ、および前記溶媒と前記非溶媒の相対的極性によって制御され、ここで、前記ポリベンズイミダゾールがスルホン化ポリベンズイミダゾールである、請求項1に記載の方法。
- 前記第1の層が範囲0.1〜10μmの厚さを有し、前記第2の層は10〜500μmの範囲の厚さを有し、前記ポリマーの析出は、落下中に部分的に固化し、クエンチング中に完全に固化する、請求項1に記載の方法。
- 繊維の壁を形成する第1および第2の同心層を含む非対称中空繊維であって、前記非対称中空繊維はポリベンズイミダゾール材料を含み、
前記第1の層は非多孔性であり、
前記第2の層は範囲5〜250nmの細孔を有する多孔性であり、
前記第1の層の化学組成と前記第2の層の化学組成が同じであり、
前記非対称中空繊維は範囲100〜2000μmの外径を有する、該非対称中空繊維。 - (a)前記ポリベンズイミダゾールがスルホン化ポリベンズイミダゾールである、または
(b)400℃まで化学分解に対して安定である、または
(c)前記第1の層が範囲0.1〜10μmの厚さを有し、前記第2の層は10〜500μmの範囲の厚さを有する、請求項9に記載の非対称中空繊維。 - 前記第1の層が前記非対称中空繊維の外表面を形成し、前記第2の層が前記非対称中空繊維の内表面を形成する、請求項9に記載の非対称中空繊維。
- 請求項9に記載の前記非対称中空繊維を繊維束中に含む膜。
- H2、CO2、COおよびメタンを含むガス混合物からH2を分離する方法であって、請求項12に記載の前記膜にガス混合物を通す工程を含む方法。
- 水溶液から不純物を除去する方法であって、請求項12に記載の前記膜に前記水溶液を通す工程を含む方法。
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US201161531448P | 2011-09-06 | 2011-09-06 | |
US61/531,448 | 2011-09-06 | ||
PCT/US2012/054033 WO2013036693A2 (en) | 2011-09-06 | 2012-09-06 | Process for fabricating pbi hollow fiber asymmetric membranes for gas separation and liquid separation |
Publications (2)
Publication Number | Publication Date |
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JP2014527906A JP2014527906A (ja) | 2014-10-23 |
JP6062945B2 true JP6062945B2 (ja) | 2017-01-18 |
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JP2014528706A Active JP6062945B2 (ja) | 2011-09-06 | 2012-09-06 | 気体分離および液体分離用のpbi中空繊維非対称膜を製作するプロセス |
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JP (1) | JP6062945B2 (ja) |
KR (1) | KR101951065B1 (ja) |
CN (1) | CN103781536B (ja) |
WO (1) | WO2013036693A2 (ja) |
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KR20230131140A (ko) | 2022-03-04 | 2023-09-12 | 한국화학연구원 | 보호기가 도입된 폴리벤즈이미다졸, 이를 이용한 막의 제조방법 및 이의 용도 |
Family Cites Families (9)
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US5762798A (en) * | 1991-04-12 | 1998-06-09 | Minntech Corporation | Hollow fiber membranes and method of manufacture |
SG94705A1 (en) * | 1998-06-16 | 2003-03-18 | Univ Singapore | Ultrathin high-performance hollow fiber membranes |
US6921482B1 (en) * | 1999-01-29 | 2005-07-26 | Mykrolis Corporation | Skinned hollow fiber membrane and method of manufacture |
US6623639B2 (en) * | 1999-03-19 | 2003-09-23 | Bend Research, Inc. | Solvent-resistant microporous polybenzimidazole membranes |
CA2300519C (en) | 1999-03-19 | 2008-02-12 | Bend Research, Inc. | Solvent-resistant microporous polybenzimidazole membranes |
KR100644366B1 (ko) * | 2005-11-08 | 2006-11-10 | 한국화학연구원 | 비대칭 기체분리용 고분자 중공사막의 대량 제조방법 |
US20110311745A1 (en) | 2008-12-16 | 2011-12-22 | National University Of Singapore | Chemically-modified polybenzimidazole membranous tubes |
CN101642683B (zh) * | 2009-09-10 | 2012-05-02 | 苏州信望膜技术有限公司 | 双层复合中空纤维纳滤膜及其制备方法和专用工具 |
CN101844040A (zh) * | 2010-06-07 | 2010-09-29 | 苏州信望膜技术有限公司 | 一种中空纤维纳滤膜及其制备方法 |
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- 2012-09-06 WO PCT/US2012/054033 patent/WO2013036693A2/en active Application Filing
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