JP6389490B2 - 触媒製造方法 - Google Patents
触媒製造方法 Download PDFInfo
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- JP6389490B2 JP6389490B2 JP2016162239A JP2016162239A JP6389490B2 JP 6389490 B2 JP6389490 B2 JP 6389490B2 JP 2016162239 A JP2016162239 A JP 2016162239A JP 2016162239 A JP2016162239 A JP 2016162239A JP 6389490 B2 JP6389490 B2 JP 6389490B2
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- metal
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- 239000003054 catalyst Substances 0.000 title claims description 80
- 238000004519 manufacturing process Methods 0.000 title claims description 18
- 238000000034 method Methods 0.000 claims description 63
- 239000000463 material Substances 0.000 claims description 48
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- 229910052751 metal Inorganic materials 0.000 claims description 32
- 239000002184 metal Substances 0.000 claims description 32
- 238000000465 moulding Methods 0.000 claims description 23
- 239000011230 binding agent Substances 0.000 claims description 15
- 150000002736 metal compounds Chemical class 0.000 claims description 13
- 239000000203 mixture Substances 0.000 claims description 13
- 239000007789 gas Substances 0.000 claims description 12
- 230000008569 process Effects 0.000 claims description 12
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 11
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 claims description 9
- 238000010438 heat treatment Methods 0.000 claims description 9
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 8
- 230000003647 oxidation Effects 0.000 claims description 8
- 238000007254 oxidation reaction Methods 0.000 claims description 8
- 229910021536 Zeolite Inorganic materials 0.000 claims description 7
- 239000000654 additive Substances 0.000 claims description 7
- 230000000996 additive effect Effects 0.000 claims description 7
- 238000000149 argon plasma sintering Methods 0.000 claims description 7
- 238000006722 reduction reaction Methods 0.000 claims description 7
- 239000010457 zeolite Substances 0.000 claims description 7
- 230000003197 catalytic effect Effects 0.000 claims description 6
- 229910044991 metal oxide Inorganic materials 0.000 claims description 6
- 150000004706 metal oxides Chemical class 0.000 claims description 6
- 239000002245 particle Substances 0.000 claims description 6
- 239000000377 silicon dioxide Substances 0.000 claims description 6
- 150000003623 transition metal compounds Chemical class 0.000 claims description 6
- 238000002485 combustion reaction Methods 0.000 claims description 5
- 229910052741 iridium Inorganic materials 0.000 claims description 5
- 229910052763 palladium Inorganic materials 0.000 claims description 5
- 229910052697 platinum Inorganic materials 0.000 claims description 5
- 230000009467 reduction Effects 0.000 claims description 5
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 4
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 4
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 4
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 4
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 4
- 229910052742 iron Inorganic materials 0.000 claims description 4
- 229910000510 noble metal Inorganic materials 0.000 claims description 4
- 229910052702 rhenium Inorganic materials 0.000 claims description 4
- 229910052707 ruthenium Inorganic materials 0.000 claims description 4
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims description 4
- 229910010271 silicon carbide Inorganic materials 0.000 claims description 4
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 4
- 229910000323 aluminium silicate Inorganic materials 0.000 claims description 3
- 229910052787 antimony Inorganic materials 0.000 claims description 3
- 229910052791 calcium Inorganic materials 0.000 claims description 3
- NKCVNYJQLIWBHK-UHFFFAOYSA-N carbonodiperoxoic acid Chemical compound OOC(=O)OO NKCVNYJQLIWBHK-UHFFFAOYSA-N 0.000 claims description 3
- 229910052804 chromium Inorganic materials 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 229910052737 gold Inorganic materials 0.000 claims description 3
- 229910052745 lead Inorganic materials 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 229910052748 manganese Inorganic materials 0.000 claims description 3
- 229910052750 molybdenum Inorganic materials 0.000 claims description 3
- 229910052759 nickel Inorganic materials 0.000 claims description 3
- 229910052758 niobium Inorganic materials 0.000 claims description 3
- 229910052700 potassium Inorganic materials 0.000 claims description 3
- 229910052703 rhodium Inorganic materials 0.000 claims description 3
- 238000007493 shaping process Methods 0.000 claims description 3
- 229910052710 silicon Inorganic materials 0.000 claims description 3
- 229910052709 silver Inorganic materials 0.000 claims description 3
- 229910052708 sodium Inorganic materials 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- 229910052719 titanium Inorganic materials 0.000 claims description 3
- 229910052721 tungsten Inorganic materials 0.000 claims description 3
- 229910052720 vanadium Inorganic materials 0.000 claims description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 3
- 229910052727 yttrium Inorganic materials 0.000 claims description 3
- 229910052725 zinc Inorganic materials 0.000 claims description 3
- 239000011701 zinc Substances 0.000 claims description 3
- 229910052726 zirconium Inorganic materials 0.000 claims description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 2
- 150000004645 aluminates Chemical class 0.000 claims description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 claims description 2
- 239000011787 zinc oxide Substances 0.000 claims description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims 1
- 239000003546 flue gas Substances 0.000 claims 1
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 10
- 239000012254 powdered material Substances 0.000 description 8
- 229910021529 ammonia Inorganic materials 0.000 description 5
- 239000012530 fluid Substances 0.000 description 5
- -1 lanthanide metal compound Chemical class 0.000 description 5
- 238000005453 pelletization Methods 0.000 description 5
- 238000006243 chemical reaction Methods 0.000 description 4
- 238000013461 design Methods 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- 239000007787 solid Substances 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 3
- 238000006555 catalytic reaction Methods 0.000 description 3
- 239000000919 ceramic Substances 0.000 description 3
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- 238000002407 reforming Methods 0.000 description 3
- 238000001179 sorption measurement Methods 0.000 description 3
- 238000003786 synthesis reaction Methods 0.000 description 3
- GQPLMRYTRLFLPF-UHFFFAOYSA-N Nitrous Oxide Chemical compound [O-][N+]#N GQPLMRYTRLFLPF-UHFFFAOYSA-N 0.000 description 2
- 241000233805 Phoenix Species 0.000 description 2
- 229910052768 actinide Inorganic materials 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 238000001354 calcination Methods 0.000 description 2
- 239000011575 calcium Substances 0.000 description 2
- 239000006185 dispersion Substances 0.000 description 2
- 238000005516 engineering process Methods 0.000 description 2
- 239000000835 fiber Substances 0.000 description 2
- 230000004927 fusion Effects 0.000 description 2
- 230000005484 gravity Effects 0.000 description 2
- 229910052747 lanthanoid Inorganic materials 0.000 description 2
- 229910052987 metal hydride Inorganic materials 0.000 description 2
- 150000004681 metal hydrides Chemical class 0.000 description 2
- 229910003455 mixed metal oxide Inorganic materials 0.000 description 2
- 239000000178 monomer Substances 0.000 description 2
- 239000013618 particulate matter Substances 0.000 description 2
- 229920000642 polymer Polymers 0.000 description 2
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- 238000001694 spray drying Methods 0.000 description 2
- 238000000629 steam reforming Methods 0.000 description 2
- 229910052723 transition metal Inorganic materials 0.000 description 2
- 229910000314 transition metal oxide Inorganic materials 0.000 description 2
- 150000003624 transition metals Chemical class 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- 150000001242 acetic acid derivatives Chemical class 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 238000013459 approach Methods 0.000 description 1
- 229910052785 arsenic Inorganic materials 0.000 description 1
- RQNWIZPPADIBDY-UHFFFAOYSA-N arsenic atom Chemical compound [As] RQNWIZPPADIBDY-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000002453 autothermal reforming Methods 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- XFWJKVMFIVXPKK-UHFFFAOYSA-N calcium;oxido(oxo)alumane Chemical compound [Ca+2].[O-][Al]=O.[O-][Al]=O XFWJKVMFIVXPKK-UHFFFAOYSA-N 0.000 description 1
- MMCOUVMKNAHQOY-UHFFFAOYSA-N carbonoperoxoic acid Chemical class OOC(O)=O MMCOUVMKNAHQOY-UHFFFAOYSA-N 0.000 description 1
- 238000001193 catalytic steam reforming Methods 0.000 description 1
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- 239000001913 cellulose Substances 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 229910052878 cordierite Inorganic materials 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000008021 deposition Effects 0.000 description 1
- JSKIRARMQDRGJZ-UHFFFAOYSA-N dimagnesium dioxido-bis[(1-oxido-3-oxo-2,4,6,8,9-pentaoxa-1,3-disila-5,7-dialuminabicyclo[3.3.1]nonan-7-yl)oxy]silane Chemical compound [Mg++].[Mg++].[O-][Si]([O-])(O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2)O[Al]1O[Al]2O[Si](=O)O[Si]([O-])(O1)O2 JSKIRARMQDRGJZ-UHFFFAOYSA-N 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
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- 150000004675 formic acid derivatives Chemical class 0.000 description 1
- 150000004676 glycans Chemical class 0.000 description 1
- 229920000591 gum Polymers 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 229910001385 heavy metal Inorganic materials 0.000 description 1
- 239000002638 heterogeneous catalyst Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 238000005984 hydrogenation reaction Methods 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 description 1
- 229910052753 mercury Inorganic materials 0.000 description 1
- 229910001960 metal nitrate Inorganic materials 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 239000001272 nitrous oxide Substances 0.000 description 1
- 239000011368 organic material Substances 0.000 description 1
- 150000003891 oxalate salts Chemical class 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000012856 packing Methods 0.000 description 1
- 238000002161 passivation Methods 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N phenol group Chemical group C1(=CC=CC=C1)O ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 229920005596 polymer binder Polymers 0.000 description 1
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- 150000003464 sulfur compounds Chemical class 0.000 description 1
- 238000012546 transfer Methods 0.000 description 1
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- 229910000859 α-Fe Inorganic materials 0.000 description 1
Classifications
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- B01D—SEPARATION
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- B01D53/02—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 adsorption, e.g. preparative gas chromatography
- B01D53/04—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 adsorption, e.g. preparative gas chromatography with stationary adsorbents
- B01D53/0407—Constructional details of adsorbing systems
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- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/86—Catalytic processes
- B01D53/8621—Removing nitrogen compounds
- B01D53/8634—Ammonia
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Description
(i)粉末化触媒又は触媒担体材料の層を形成し、
(ii)予め定められたパターンに従って上記層中の粉末を結合又は融合させ、
(iii)(i)及び(ii)を繰り返して何層も重ねて成形ユニットを形成し、
(iv)場合によっては上記成形ユニットに触媒材料を適用する
工程を含む方法を提供する。
好ましくは、成形ユニットは、断面が円形、楕円形又は多角形、例えば三角形、正方形、長方形又は六角形であってもよい一又は複数の貫通孔を有する。貫通孔は成形ユニットの長軸に対して、平行に走る二以上の貫通孔、又は様々な角度で成形ユニットを貫通して走る非平行の孔を含みうる。一般的なペレット化及び押出技術を使用すると現在はできない、湾曲した貫通孔もまたALM法を使用して作製することができる。
触媒が金属粉末である場合、好ましくは金属粉末は、場合によっては一又は複数の遷移金属と混合されて、例えばPt、Pd、Ir、Ru、Reの一又は複数を含む貴金属触媒粉末を含む。
あるいは、触媒粉末はゼオライトを含みうる。
あるいは、触媒担体粉末はゼオライトを含みうる。
成形ユニットに塗布される触媒材料は金属、金属化合物又はゼオライトを含みうる。
バーンアウト添加剤を触媒粉末又はバインダーに含めて、得られる成形ユニットの孔隙率を制御してもよい。
ALM法を使用して調製される触媒は、反応物質混合物が触媒反応を行わしめる条件下で触媒成形ユニットと接触させる。あるいは、成形ユニットが収着プロセスにおいて使用され、液体又は気体でありうるプロセス流体から物質を触媒的に除去されうる。
図1に図示したワイヤフレームアンモニア酸化触媒を、市販のペレット化アンモニア酸化触媒と比較した。
図1に係る成形ユニットにおける有効面積はおよそ545mm2である。形状体積はおよそ135mm3である。充填体積はおよそ90mm3と推定される。
これを元にすると、同じ操作条件下で同じ変換効率が一般的なペレットの数の15−16%で得られうることが予想される。
図2の12面体フレーム構造を、Phenix Systems PXシリーズのレーザー焼結機を使用して調製した。およそ10ミクロンの平均粒径の未変性アルミナ粉末を用い、レーザー溶融前にそれぞれの新粉末層を圧密化し、およそ100ミクロンのステップを使用して、ビルドが達成された。300Wのファイバーレーザーを使用し、標準的なソフトウェアによって駆動されるトラックに沿ってアルミナを溶融させた。ビルド完了時は部品は壊れやすく、粉末床から注意して取り除いた。強度の増強は約1800℃までの温度でのビルド後焼結によって達成されうる。
図3のアルミナ−シリカ12面体形状の「3Dプリンティング」を、Z−Corp 3Dプリンターと標準的な市販の結合媒を使用して達成した。中央値がおよそ30ミクロンの粒径の粉末を、常套的な加工条件を使用して100ミクロンステップでプリントした。製造した未焼結(green)構造体を、およそ8時間にわたってゆっくりした温度の立ち上がりとしておよそ1000℃まで燃やし続け、結合剤を燃やして除去し、完全な状態を損ねないで部品を緻密化(収縮)させた。完了時に、十分に強く触媒コーティングに耐える多量の3D形状体が製造された。
Claims (16)
- 内燃機関の排気ガスの成分の選択的酸化又は還元のための、触媒モノリス成形ユニットの製造方法であって、触媒モノリス成形ユニットが添加剤層法を含む方法によって得られ、該方法は以下の工程:
(i)粉末化触媒材料又は粉末化触媒担体材料の層を形成する工程;
(ii)予め定められたパターンに従って層中の粉末化触媒材料又は粉末化触媒担体材料を結合又は融合させる工程;
(iii)(i)及び(ii)を繰り返して何層も重ねてモノリスを形成する工程;及び
(iv)粉末化触媒担体材料から形成されたモノリスにおいて、触媒担体材料に触媒材料を適用する工程;
を含み、
粉末化触媒材料又は工程(iv)においてモノリスの触媒担体材料に適用される触媒材料が、Na、K、Mg、Ca、Ba、Al、Si、Ti、V、Cr、Mn、Fe、Co、Ni、Cu、Zn、Y、Zr、Nb、Mo、Ru、Rh、Pd、Ag、Sn、Sb、La、Hf、W、Re、Ir、Pt、Au、Pb、又はCeからなる群から選択される金属を含む一又は複数の金属又は金属化合物を含み、
成形ユニットは、100−1000mmの範囲の断面を有する、
触媒モノリス成形ユニットの製造方法。 - 粉末化触媒材料が、一又は複数のPt、Pd、Ir、Ru、Rh又はReを含む貴金属触媒粉末を含む、請求項1に記載の方法。
- 粉末化触媒材料が、金属酸化物、金属水酸化物、金属炭酸塩、金属ヒドロキシ炭酸塩又はその混合物から選択される遷移金属化合物を含む、請求項1又は2に記載の方法。
- 粉末化触媒材料が一又は複数の不活性材料を含む、請求項1から3の何れか一項に記載の方法。
- 一又は複数の不活性材料が、アルミナ、シリカ、窒化珪素、炭化珪素、炭素及びそれらの混合物からなる群から選択される、請求項4に記載の方法。
- 粉末化触媒材料がゼオライトを含む、請求項1に記載の方法。
- 触媒担体材料がアルミナ、金属アルミネート、シリカ、アルミノ-シリケート、窒化珪素、炭化珪素、チタニア、炭素、ジルコニア、亜鉛酸化物、及びそれらの混合物からなる群から選択される一又は複数の不活性材料を含む、請求項1に記載の方法。
- 触媒担体材料が、一又は複数の金属酸化物、金属水酸化物、金属炭酸塩、金属ヒドロキシ炭酸塩又はそれらの混合物から選択される、一又は複数の遷移金属化合物を含む、請求項1に記載の方法。
- 粉末化触媒担体材料がゼオライトを含む、請求項1に記載の方法。
- 粉末化触媒材料又は粉末化触媒担体材料が1から200マイクロメートルの平均粒径を有する、請求項1から9の何れか一項に記載の方法。
- 触媒モノリス成形ユニットがハニカムモノリスである、請求項1から10の何れか一項に記載の方法。
- 添加剤層法が3Dプリンティング、ステレオリソグラフィー又はレーザ焼結法を含む、請求項1から11の何れか一項に記載の方法。
- 各層の粉末がバインダーと共に結合される、請求項12に記載の方法。
- モノリス成形ユニットが加熱工程に供される、請求項12又は13に記載の方法。
- 内燃機関の排ガスの選択的酸化又は還元反応を触媒するための請求項1から11の何れか一項に記載の方法によって得られる触媒モノリス成形ユニットの使用。
- モノリス成形ユニットのアスペクト比が0.5から5の範囲である、請求項1から14の何れか一項に記載の方法。
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US20130230721A1 (en) | 2013-09-05 |
EP2752244A1 (en) | 2014-07-09 |
WO2012032325A1 (en) | 2012-03-15 |
EP2613879A1 (en) | 2013-07-17 |
US20150360207A1 (en) | 2015-12-17 |
EP2752244B1 (en) | 2021-01-27 |
EP2613879B2 (en) | 2024-02-14 |
AU2011300512B2 (en) | 2017-02-02 |
CN103118782A (zh) | 2013-05-22 |
CN105195235A (zh) | 2015-12-30 |
AU2011300512A1 (en) | 2013-05-02 |
GB201014950D0 (en) | 2010-10-20 |
US20160136634A1 (en) | 2016-05-19 |
RU2016134735A3 (ja) | 2019-12-04 |
RU2013115444A (ru) | 2014-10-20 |
RU2016134735A (ru) | 2018-12-11 |
CN105107551A (zh) | 2015-12-02 |
BR112013004969A2 (pt) | 2016-08-16 |
RU2598381C2 (ru) | 2016-09-27 |
US9839907B2 (en) | 2017-12-12 |
CN103118782B (zh) | 2015-11-25 |
US9272264B2 (en) | 2016-03-01 |
US9278338B2 (en) | 2016-03-08 |
JP2013537847A (ja) | 2013-10-07 |
US20170189897A1 (en) | 2017-07-06 |
JP2017029981A (ja) | 2017-02-09 |
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