JP6983480B2 - 改善された品質の減圧残油生成物を生成するための沸騰床改良用二元触媒システム - Google Patents
改善された品質の減圧残油生成物を生成するための沸騰床改良用二元触媒システム Download PDFInfo
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- JP6983480B2 JP6983480B2 JP2018563559A JP2018563559A JP6983480B2 JP 6983480 B2 JP6983480 B2 JP 6983480B2 JP 2018563559 A JP2018563559 A JP 2018563559A JP 2018563559 A JP2018563559 A JP 2018563559A JP 6983480 B2 JP6983480 B2 JP 6983480B2
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
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- C10G45/02—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing
- C10G45/04—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to eliminate hetero atoms without changing the skeleton of the hydrocarbon involved and without cracking into lower boiling hydrocarbons; Hydrofinishing characterised by the catalyst used
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
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- C10G45/44—Hydrogenation of the aromatic hydrocarbons
- C10G45/46—Hydrogenation of the aromatic hydrocarbons characterised by the catalyst used
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
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- C10G47/02—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions characterised by the catalyst used
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G47/00—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions
- C10G47/24—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions with moving solid particles
- C10G47/26—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions with moving solid particles suspended in the oil, e.g. slurries
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
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- C10G49/26—Controlling or regulating
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- C—CHEMISTRY; METALLURGY
- C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
- C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
- C10G65/00—Treatment of hydrocarbon oils by two or more hydrotreatment processes only
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Description
この出願の発明に関連する先行技術文献情報としては、以下のものがある(国際出願日以降国際段階で引用された文献及び他国に国内移行した際に引用された文献を含む)。
(先行技術文献)
(特許文献)
(特許文献1) 米国特許出願公開第2013/0233765号明細書
(特許文献2) 米国特許第5,309,537号明細書
(特許文献3) 米国特許出願公開第2012/0152605号明細書
(特許文献4) 米国特許出願公開第201310228494号明細書
(特許文献5) 米国特許出願公開第2014/0291203号明細書
(特許文献6) 米国特許第 5,858,923号明細書
(非特許文献)
(非特許文献1) Rana el al.,A review or recent advances on process technologies for upgrading of heavy oils and residua,7 September 2008,tult text,retrieved from http://www.sciencedireet.com/science/article/pii/S001623610GOD295X on B August 2017
本発明は、沸騰床水素処理システムにおいて二元触媒システムを用いて、重油から転化された炭化水素転化生成物および改善された品質の減圧残油生成物を生成する方法およびシステムに関する。この方法およびシステムは、固体担持(すなわち不均一な)触媒と、十分に分散した(すなわち均質な)触媒粒子とからなるを有する2元触媒システムを用いるものに関する。前記二元触媒システムは、通常ならば固体担持沸騰床触媒から成る単一の触媒を用いた沸騰床水素処理システムを改良するのに用いることができる。
図2A〜2Dは、重油などの炭化水素原料を水素処理するのに用いられる沸騰床水素処理反応器およびシステムの非限定的な例を概略的に示したものであり、当該反応器およびシステムは本発明において二元触媒を用いるように改良され得る。この例示的な沸騰床水素処理反応器およびシステムは、段間分離、一体化された水素化精製および/または一体化された水素化分解を含むことができることを理解されよう。
図3A、図3B、図3Cおよび図3Dは、二元触媒システムを用い、(例えば、粘度の低下、比重の低下、アスファルテン含有量の減少、炭素含有量の減少、硫黄含有量の減少、および沈降物含有量の減少のうちの1若しくはそれ以上によって測定される)改善された品質の減圧残油生成物を生成するように沸騰床反応器を改良する例示的な方法を示すフローダイアグラムである。
図3Dは、方法であって、(1)不均一触媒を用いて初期条件で重油を水素処理するように沸騰床反応器を初期的に稼働し、初期品質の減圧残油を生成する工程と、(2)分散金属硫化物触媒粒子を前記沸騰床反応器に添加して、不均一触媒と前記分散金属硫化物触媒粒子とを含む二元触媒システムを有する改良された反応器を形成する工程と、(3)前記二元触媒システムを用いて前記改良された沸騰床反応器を同等又はより高い酷度、スループットおよび/または転化率で稼働し、初期条件で稼働している時よりも改善された品質の減圧残油生成物を生成する工程とを有する方法を示すフローダイアグラムである。
図4は、本明細書に開示される方法およびシステムで用いられる改良された沸騰床水素処理システム400の一例を概略的に示す。沸騰床水素処理システム400は、改良された沸騰床反応器430と、高温分離器404(または蒸留塔のようなその他の分離器)とを含む。改良された沸騰床反応器430を形成するために、触媒前駆体402がまず1若しくはそれ以上の混合器406中で炭化水素希釈剤404と予混合されて、触媒前駆体混合物409を形成する。触媒前駆体混合物409は原料408に添加され、1若しくはそれ以上の混合器410において原料と混合されて、調整済み原料411を形成する。調整済み原料は周辺ポンプ414を伴うサージ容器412に供給されて、調整済み原料内において触媒前駆体の更なる混合および分散がもたらされる。
本明細書に開示されるように、二元触媒システムを用いるように沸騰床水素処理システムを改良することは、重油を改良し、より軽くより価値の高い留分を除去した後に残る減圧残油の品質を実質的に改善し得る。改善された品質の減圧残油生成物は、粘度、比重(増加したAPI比重)、アスファルテン含有量、炭素含有量、硫黄含有量、および沈降物含有量の1若しくはそれ以上の減少によって特徴付けられる。
‐ウラル減圧残油原料の場合、40〜50%;
‐アラブミディウム減圧残油原料の場合、30〜50%;
‐アサバスカ減圧残油原料の場合、60〜70%;
‐マヤ常圧残油原料の場合、40〜50%。
‐アラブミディウム減圧残油原料の場合、〜1°API
‐アサバスカ減圧残油原料の場合、最大10°API;
‐マヤ常圧残油原料の場合、〜0.2°API。
‐ウラル減圧残油原料の場合、15〜20%(相対);
‐アラブミディウム減圧残油原料の場合、少なくとも30〜40%(相対);
‐アサバスカ減圧残油原料の場合、〜50%(相対)。
‐ウラル減圧残油原料の場合、10〜15%(相対);
‐アサバスカ減圧残油原料の場合、〜30%(相対)。
‐ウラル減圧残油原料の場合、〜30%(相対);
‐アラブミディウム減圧残油原料の場合、25−30%(相的);
‐アサバスカ減圧残油原料の場合、最大40%(相対)。
以下の試験的研究は、重油を水素処理する際に、不均一触媒と分散金属硫化物触媒粒子と有する二元触媒システムを用いるように沸騰床反応器を改良することの効果および利点を実証するものである。具体的には、この試験的研究は、本発明の利用によって達成することができる減圧残油生成物の品質の改善を実証する。この試験のために図5のようにパイロットプラントが設計された。図5に概略的に示すように、直列に接続された2つの沸騰床反応器512,512'を備えたパイロットプラント500を用いて、重油原料を処理する際に不均一触媒を単独で用いる場合と、不均一系触媒を分散金属硫化物(すなわち、分散二硫化モリブデン触媒粒子)と組み合わせたものを有する二元触媒システムを用いる場合の差を判定した。
実施例1〜6を上述のパイロットプラントで実施し、不均一触媒のみで稼働される沸騰床システムと比較して、改善された品質の減圧残油生成物を生成するように二元触媒システムを用いて改良された沸騰床反応器の能力を試験した。この一組の実施例において、重油原料は、1000°F(538℃)の公称カットポイントを有するウラル減圧残油(Ural VR)とした。上記のように、調整済み原料は、一定量の触媒前駆体混合物を一定量の重油原料と混合することによって調製して、最終的な調整済み原料が必要量の分散触媒を含有するようにした。この例外として分散触媒を用いない試験があり、その場合では、触媒前駆体混合物の代わりに同じ割合で重質減圧軽油を用いた。
実施例7〜13は、重油原料が、主にアラブミディウム減圧残油(アラブミディウムVR)を主成分とする製油所供給混合であること、また1000°F(538℃)の公称カットポイントを伴うことを除いて、実施例1〜6と同じ装置および方法を用いて実施された。整済み重油原料の調製方法は、実施例1〜6について記載した方法と同様であった。
実施例14〜19は、重油原料が975°F(524℃)の公称カットポイントを有するアサバスカ減圧残油(アサバスカVR)であったことを除いて、実施例1〜6と同じ装置および方法を用いて実施された。調整済み重油原料の調製方法は、実施例1〜6について記載した方法と同様であった。
実施例20および21は、典型的な減圧残油を燃料油の規格に適合させるのに必要な硫黄含有量およびカッターストックの量に関して、減圧残油の品質を改善することに付随する利点の更なる比較および説明を提供する。実施例20は、不均一系触媒を用いる従来式の沸騰床水素処理システムを稼働してウラル減圧残油(ウラルVR)原料から減圧塔底(VTB)生成物を生成する場合の実際の結果に基づく。実施例21は、不均一触媒および分散金属硫化物触媒粒子を含む二元触媒システムを用いて改良された沸騰床水素処理システムを稼働してウラルVR原料から改善された品質の減圧塔底(VTB)生成物を生成する場合の実際の結果に基づく。比較結果を表6に示す。
Claims (18)
- 底部生成物の品質を改善するために1若しくはそれ以上の沸騰床反応器を含む沸騰床水素処理システムを改良する方法であって、
転化生成物の初期生成速度で重油を水素処理するように、不均一触媒を用いて沸騰床反応器を初期稼働する工程と、蒸留プロセスによって前記転化生成物を1若しくはそれ以上の揮発性留分と初期品質の初期底部生成物に分離する工程であって、前記1若しくはそれ以上の揮発性留分は初期速度で生成されるものであり、および、前記初期底部生成物は初期速度で生成され、初期品質を有している、分離する工程と、
その後、分散金属硫化物触媒粒子と不均一触媒とからなる二元触媒システムを用いて稼働するように、前記沸騰床反応器を改良する工程と、
重油を水素処理するように、前記二元触媒システムを用いて前記改良された沸騰床反応器を稼働する工程であって、前記水素処理は、前記初期速度と少なくとも同等の転化生成物の生成速度をもたらす反応器酷度によって特徴付けられる、稼働する工程と、蒸留プロセスによって前記転化生成物を1若しくはそれ以上の揮発性留分と改善された底部生成物に分離する工程であって、前記反応器酷度は、前記1若しくはそれ以上の揮発性留分を、少なくとも前記初期速度と同等の速度で生成させる、分離する工程と
を有し、
前記改善された底部生成物は、初期品質の前記初期底部生成物より高い品質を有し、前記改善された底部生成物は、初期品質の前記初期底部生成物の初期粘度に比べて少なくとも10%低下した粘度を有すること、および、
初期品質の前記初期底部生成物の初期API比重に比べて増加したAPI比重、
初期品質の前記初期底部生成物の初期アスファルテン含有量に比べて減少したアスファルテン含有量、
初期品質の前記初期底部生成物の初期残留炭素含有量に比べて減少した残留炭素含有量、
初期品質の前記初期底部生成物の初期硫黄含有量に比べて減少した硫黄含有量、および、
初期品質の前記初期底部生成物の初期沈降物含有量に比べて減少した沈降物含有量
から選択される、少なくとも1つの追加のより高い品質特性を有することによって特徴付けられるものである、
方法。 - 請求項1に記載の方法において、前記重油は、重質原油、油砂瀝青、製油所プロセスからの残留物、ビスブレーカ底部物、少なくとも343℃(650°F)の公称沸点を有する常圧塔底物、少なくとも524℃(975°F)の公称沸点を有する減圧塔底物、高温分離器からの残油、残留ピッチ、溶媒脱アスファルト化による生成物、または減圧残油のうちの少なくとも1つを有する、方法。
- 請求項1又は2に記載の方法において、前記蒸留プロセスは減圧蒸留であり、および、前記底部生成物は減圧塔底生成物(減圧残油生成物)である、方法。
- 請求項1又は2に記載の方法において、前記蒸留プロセスは常圧蒸留であり、および、前記底部生成物は常圧塔底生成物(常圧残油生成物)である、方法。
- 請求項1〜4のいずれか1つに記載の方法において、前記改良された沸騰床反応器によって生成され、前記1若しくはそれ以上の揮発性留分から分離された前記改善された底部生成物は、初期品質の前記初期底部生成物の初期粘度に対して、少なくとも25%、または少なくとも40%減少した粘度を有する、方法。
- 請求項1〜5のいずれか1つに記載の方法において、前記改良された沸騰床反応器によって生成され、前記1若しくはそれ以上の揮発性留分から分離された前記改善された底部生成物は、初期品質の前記初期底部生成物の初期API比重に対して、少なくとも0.1度、または少なくとも0.5度、または少なくとも1度増加したAPI比重を有する、方法。
- 請求項1〜6のいずれか1つに記載の方法において、前記改良された沸騰床反応器によって生成され、前記1若しくはそれ以上の揮発性留分から分離された前記改善された底部生成物は、初期品質の前記初期底部生成物の初期アスファルテン含有量に対して、少なくとも10%、または少なくとも20%、または少なくとも30%減少したアスファルテン含有量を有する、方法。
- 請求項1〜7のいずれか1つに記載の方法において、前記改良された沸騰床反応器によって生成され、前記1若しくはそれ以上の揮発性留分から分離された前記改善された底部生成物は、初期品質の前記初期底部生成物の初期残留炭素含有量に対して、少なくとも5%、または少なくとも10%、または少なくとも20%減少した残留炭素含有量を有する、方法。
- 請求項1〜8のいずれか1つに記載の方法において、前記改良された沸騰床反応器によって生成され、前記1若しくはそれ以上の揮発性留分から分離された前記改善された底部生成物は、初期品質の前記初期底部生成物の初期硫黄含有量に対して、少なくとも10%、または少なくとも20%、または少なくとも30%減少した硫黄含有量を有する、方法。
- 請求項1〜9のいずれか1つに記載の方法において、前記改良された沸騰床反応器によって生成され、前記1若しくはそれ以上の揮発性留分から分離された前記改善された底部生成物は、初期品質の前記初期底部生成物の初期沈降物含有量に対して、少なくとも5%、または少なくとも10%、または少なくとも20%減少した沈降物含有量を有する、方法。
- 請求項1〜10のいずれか1つに記載の方法において、前記分散金属硫化物触媒粒子は、1μm未満のサイズ、または500nm未満のサイズ、または100nm未満のサイズ、または25nm未満のサイズ、または10nm未満のサイズである、方法。
- 請求項11に記載の方法において、前記分散金属硫化物触媒粒子は、触媒前駆体から前記重油中においてその場で形成されるものであり、前記方法はさらに、前記触媒前駆体を希釈剤炭化水素と混合して希釈された前駆体混合物を形成する工程と、前記希釈された前駆体混合物を前記重油と混合して調整された重油を形成する工程と、前記調整された重油を加熱して前記触媒前駆体を分解し、かつその場で前記分散金属硫化物触媒粒子を形成する工程とを有するものである、方法。
- 請求項1〜12のいずれか1つに記載の方法において、前記改良された沸騰床反応器を稼働する工程は、前記沸騰床反応器を初期的に稼働するときと同等またはそれより高い酷度で稼働する工程によって特徴付けられるものであり、前記同等またはそれより高い酷度で稼働する工程は、
前記沸騰床反応器を初期的に稼働するときと同等またはそれより高いスループットで稼働する工程、
前記沸騰床反応器を初期的に稼働するときと同等またはそれより高い温度で稼働する工程、または、
前記沸騰床反応器を初期的に稼働するときと同等またはそれより高い転化率で稼働する工程、
の少なくとも1つによって特徴付けられるものである、方法。 - 底部生成物の品質を改善するために1若しくはそれ以上の沸騰床反応器を含む沸騰床水素処理システムを改良する方法であって、
初期酷度および転化生成物の初期生成速度で重油を水素処理するように、不均一触媒を用いて沸騰床反応器を初期稼働する工程と蒸留プロセスによって前記転化生成物を1若しくはそれ以上の揮発性留分と初期品質の初期底部生成物に分離する工程であって、前記1若しくはそれ以上の揮発性留分は初期速度で生成され、および、前記初期底部生成物は初期速度で生成され、初期品質を有している、分離する工程と、
その後、分散金属硫化物触媒粒子と不均一触媒とからなる二元触媒システムを用いて稼働するように、前記沸騰床反応器を改良する工程と、
酷度および転化生成物の生成速度が前記初期酷度および前記初期速度よりも高い状態で重油を水素処理するように、前記二元触媒システムを用いて前記改良された沸騰床反応器を稼働する工程と、蒸留プロセスによって前記転化生成物を1若しくはそれ以上の揮発性留分と改善された底部生成物に分離する工程であって、前記酷度は、前記1若しくはそれ以上の揮発性留分を、少なくとも前記初期速度と同等の速度で生成させる、分離する工程と
を有し、
前記改善された底部生成物は、前記初期品質の前記初期底部生成物と同等またはより高い品質を有し、前記改善された底部生成物は、初期品質の前記初期底部生成物の粘度と同じか、それよりも低下した粘度を有すること、および、
初期品質の前記初期底部生成物の初期アスファルテン含有量と同じか、それよりも低下したアスファルテン含有量、
初期品質の前記初期底部生成物の初期残留炭素含有量と同じか、それよりも低下した残留炭素含有量、
初期品質の前記初期底部生成物の初期硫黄含有量と同じか、それよりも低下した硫黄含有量、
初期品質の前記初期底部生成物の初期API比重と同じか、それよりも高いAPI比重、または、
初期品質の前記初期底部生成物の初期沈降物含有量と同じか、それよりも低下した沈降物含有量、
から選択される、少なくとも1つの追加の同等またはより高い品質特性を有することによって特徴付けられるものである、方法。 - 請求項14に記載の方法において、前記蒸留プロセスは減圧蒸留であり、および、前記底部生成物は減圧塔底生成物(減圧残油生成物)である、方法。
- 請求項14に記載の方法において、前記蒸留プロセスは常圧蒸留であり、および、前記底部生成物は常圧塔底生成物(常圧残油生成物)である、方法。
- 請求項15または16に記載の方法において、前記1若しくはそれ以上の揮発性留分をより高い速度で生成するように前記改良された沸騰床をより高い酷度および転化生成物の生成速度より高い生成速度で稼働する工程は、前記初期底部生成物の前記初期生成速度よりも低い速度で生成される前記改善された底部生成物をもたらし、前記より高い酷度は、
同等のスループットを維持しながら、より高い温度およびより高い転化率で稼働する工程、
同等の転化率を維持しながら、より高いスループット、およびより高い温度で稼働する工程、または、
より高い温度、より高いスループット、およびより高い転化率で稼働する工程
によって特徴付けられるものである、方法。 - 請求項14〜17のいずれか1つに記載の方法において、前記改良された沸騰床によって生成された前記改善された底部生成物は、
前記初期品質の前記初期底部生成物の初期粘度と比較して少なくとも10%低下した粘度、
前記初期品質の前記初期底部生成物の初期アスファルテン含有量と比較して少なくとも10%低下したアスファルテン含有量、
前記初期品質の前記初期底部生成物の初期残留炭素含有量と比較して少なくとも5%低下した残留炭素含有量、
前記初期品質の前記初期底部生成物の初期硫黄含有量と比較して少なくとも10%低下した硫黄含有量、
前記初期品質の前記初期底部生成物の初期API比重と比較して少なくとも0.1度増加したAPI比重、または、
前記初期品質の前記初期底部生成物の初期沈降物含有量と比較して少なくとも5%低下した沈降物含有量、
の少なくとも1つによって特徴付けられるものである、方法。
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2017
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- 2017-06-07 CN CN201780035917.7A patent/CN109563416B/zh active Active
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US11421164B2 (en) | 2022-08-23 |
KR102414335B1 (ko) | 2022-06-29 |
EA201892721A8 (ru) | 2019-12-16 |
KR20190018465A (ko) | 2019-02-22 |
CA3025419C (en) | 2024-04-16 |
EP3469044A4 (en) | 2020-03-11 |
CA3025419A1 (en) | 2017-12-14 |
EA201892721A1 (ru) | 2019-09-30 |
JP2019521211A (ja) | 2019-07-25 |
CN109563416B (zh) | 2022-01-18 |
EP3469044A1 (en) | 2019-04-17 |
US20170355913A1 (en) | 2017-12-14 |
CN109563416A (zh) | 2019-04-02 |
WO2017214256A1 (en) | 2017-12-14 |
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