JP2023502555A - 水素富化圧縮天然ガスおよびカーボンナノチューブの同時製造 - Google Patents
水素富化圧縮天然ガスおよびカーボンナノチューブの同時製造 Download PDFInfo
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Abstract
Description
Claims (23)
- 水素富化圧縮天然ガス(H-CNG)およびカーボンナノチューブ(CNT)を同時製造するためのプロセスであって、前記プロセスが、
a.触媒が充填された第1の流動床反応器(FBR)内で反応サイクルを実施することであって、前記反応サイクルが、
i.水素ガスを含む第1のガスを使用して前記触媒を活性化させることであって、前記触媒が活性金属触媒を含む、活性化させること、
ii.前記第1のガスの通過を停止した後に炭化水素供給ガスを前記FBRに通過させること、
iii.クラッキング反応を前記FBR内で所定の時間にわたって進め、前記触媒上に堆積されたCNTを含む使用済み触媒と、H-CNGおよび同伴された使用済み触媒を含む生成物ガスとを得ること、
iv.前記生成物ガスを連続的に除去し、前記使用済み触媒を所定の時間間隔で前記FBRから除去すること、
v.前記生成物ガスをサイクロンに通過させて、前記同伴された使用済み触媒を分離し、分離された生成物ガスを得て、前記同伴された使用済み触媒を、前記FBRから除去された前記使用済み触媒と混合すること、
vi.CNTを前記使用済み触媒から分離して、生成物CNTを得ること、
vii.熱回収ユニット内で流体流と熱を交換することによって、熱を前記分離された生成物ガスから回収して、回収された生成物ガスおよび加熱された流体流を得ること、
viii.前記触媒を前記FBRに充填する前に、前記加熱された流体流を、前記触媒を調製するための活性金属触媒と触媒担体とを含む触媒反応器に通過させ、前記回収された生成物ガスの少なくとも一部を前記第1のガスとして前記FBRに通過させて、ステップ(i)で前記触媒を活性化させること、ならびに
ix.前記FBR内での前記反応を停止し、残りの使用済み触媒および生成物ガスを除去すること、を含む、実施することと、
b.前記第1のFBR内での前記反応サイクルが開始した後に、第2のFBRに前記触媒を充填し、ステップ(i~ix)を含む前記反応サイクルを第1の所定の時間で前記第2のFBR内で実施することであって、前記第2のFBRが、前記第1のFBR内での前記反応サイクルが停止された後に、第2の所定の間にわたって運転可能なままである、実施することと、
c.前記第2のFBR内での前記反応サイクルが開始した後に、前記第1のFBRに前記触媒を充填し、ステップ(i~ix)を含む前記反応サイクルを第3の所定の時間で前記第1のFBR内で実施することであって、前記第1のFBRが、前記第2のFBR内での前記反応サイクルが停止された後に、第4の所定の間にわたって運転可能なままである、実施することと、
d.H-CNGおよびCNTを連続的に同時製造するためにステップ(a~c)を繰り返すことと、を含む、プロセス。 - 前記炭化水素供給ガスを前記第1のFBRまたは前記第2のFBRに送る前に前記炭化水素供給ガスと熱を交換することによって、熱を前記使用済み触媒から回収することを含む、請求項1に記載のプロセス。
- 触媒活性化後に得られた減損した第1のガスを、前記第1のFBRまたは前記第2のFBRに送られた炭化水素ガス供給物と混合することを含み、前記減損した第1のガスは水素ガスの減損である、請求項1に記載のプロセス。
- 前記クラッキング反応が、500~750℃で10~50時間にわたって進む、請求項1に記載のプロセス。
- 生成物CNTの分離後に、前記使用済み触媒を再生し、前記第1のFBRまたは前記第2のFBRの充填のために新鮮な触媒と混合する、請求項1に記載のプロセス。
- 触媒前駆体を前記触媒反応器内で前記触媒担体上に注入しながら、前記加熱された流体流を通過させて、インサイチュで前記触媒担体において前記活性金属触媒を生成することを含む、請求項1に記載のプロセス。
- 前記加熱された流体流を通過させる前に、前記活性金属触媒を前記触媒反応器内で前記触媒担体上に堆積させることを含む、請求項1に記載のプロセス。
- 前記触媒担体が、アルミナ、バイオ炭、Yゼオライト、ZSM-5、ベータゼオライト、MFIゼオライト、モルデナイト、MgO、SiO2、使用済みFCC触媒、またはそれらの組み合わせから選択される、請求項1に記載のプロセス。
- 前記活性金属触媒が、Pt、Pd、Cu、Zr、Zn、CeO2、およびそれらの組み合わせから選択される促進剤を有するNiまたはFe系触媒である、請求項1に記載のプロセス。
- 前記炭化水素供給ガスが、圧縮天然ガス、メタン、エタン、プロパン、ブタン、エチレン、アセチレン、ナフサ、原油、ディーゼル、清浄化された油、またはそれらの組み合わせから選択される、請求項1に記載のプロセス。
- 前記第1のガスが、前記炭化水素供給ガスと混合された水素、またはH-CNGである、請求項1に記載のプロセス。
- 前記CNTを前記使用済み触媒から分離することを、酸分解法、超音波処理もしくは機械的摩砕、またはそれらの組み合わせによって実施する、請求項1に記載のプロセス。
- 熱回収のための前記流体流が、水、蒸気、窒素、炭化水素供給ガス、またはそれらの組み合わせを含む、請求項1に記載のプロセス。
- 先行請求項のいずれか一項に記載のプロセスによって水素富化圧縮天然ガス(H-CNG)およびカーボンナノチューブ(CNT)を同時製造するための装置であって、前記装置が、
a.炭化水素供給ガスタンクと、
b.少なくとも2つの流動床反応器(FBR)であって、各流動床反応器が、
シェル、
活性金属触媒を保持するために前記シェルの高さに沿って異なる高さでカンチレバーとして配設されたトレイであって、連続するトレイが、前記シェルの径方向に反対の端部に取り付けられており、各トレイが、前記トレイ上に触媒保持体積を形成するために自由端部に堰部を有する、トレイ、
前記活性金属触媒を前記トレイ上に配置することを可能にするために各トレイの上方に設けられた触媒入口、
前記炭化水素供給ガスが前記活性金属触媒の存在下で前記クラッキング反応を受けるように前記反応器に入り、前記H-CNGおよびCNTを製造することを可能にするための、各トレイの下方に設けられたガス分配器、
H-CNGを含む前記生成物ガスが前記反応器から出ることを可能にするために前記シェルの頂部に配設されたガス出口、ならびに
前記反応を停止する際にCNTを含む前記使用済み触媒を前記反応器から除去するための、前記シェルの底部に配設された触媒出口、を備える、流動床反応器(FBR)と、
c.熱を前記生成物ガスから回収し、前記加熱された流体流を生成するための熱回収ユニットと、
d.触媒調製のための、前記触媒担体、活性金属触媒、および前記加熱された流体流を収容するための触媒反応器と、
e.生成物CNTを収集するためのCNT収集器と、を備える、装置。 - 水素富化圧縮天然ガス(H-CNG)およびカーボンナノチューブ(CNT)を同時製造するための流動床反応器(FBR)であって、前記反応器が、
シェル、
活性金属触媒を保持するために前記シェルの高さに沿って異なる高さで配設されたトレイであって、前記トレイの直径が前記シェルの直径よりも小さく、そのため、前記トレイの自由端部と前記シェルの内側表面との間に通路が形成されている、トレイ、
前記活性金属触媒を前記トレイ上に配置することを可能にするために前記シェル上に設けられた触媒入口、
前記炭化水素供給ガスが前記活性金属触媒の存在下でクラッキング反応を受けるように前記反応器に入り、H-CNGおよびCNTを製造することを可能にするための、前記シェルに取り付けられたガス分配器、
H-CNGを含む生成物ガスが前記反応器から出ることを可能にするために前記シェルの頂部に配設されたガス出口、ならびに
CNTを含む使用済み触媒を前記反応器から除去するための、前記シェルの底部に配設された触媒出口、を備える、流動床反応器(FBR)。 - 前記トレイが片方の端部で前記シェルに固定されて、カンチレバーを形成している、請求項15に記載のFBR。
- より高いトレイからの触媒が前記通路を通ってより低いトレイに落下することを可能にし、かつ反応物および生成物ガスが前記通路を通って上昇する直線経路の形成を防ぐために、連続するトレイが、前記シェルの径方向に反対の端部で前記シェルに固定されている、請求項15に記載のFBR。
- 各トレイ上に触媒保持体積を形成して各トレイ上に個々の流動床を形成するために、堰部が各前記トレイの自由端部上に配設されている、請求項15に記載のFBR。
- 前記堰部の高さが様々である、請求項18に記載のFBR。
- 反応物および生成物ガスの流れが、前記トレイを通過して、その上に配置されている前記活性金属触媒を流動化させ、クラッキング反応を進めることを可能にするために、前記トレイが、前記トレイの基部に設けられた開口部を備える、請求項15に記載のFBR。
- 使用済み触媒を前記トレイから除去することを可能にするさらなる使用済み触媒出口を備える、請求項15に記載のFBR。
- 反応器本体を備え、前記トレイ、触媒入口、ガス分配器、ガス出口、および触媒出口を有するシェルが一体型反応器ユニットとして形成されており、前記一体型反応器ユニットが前記反応器本体に取り外し可能に配設されている、請求項15に記載のFBR。
- 触媒入口が各トレイに隣接してかつその上方に設けられており、ガス分配器が各トレイに隣接してかつその下方に設けられている、請求項15に記載のFBR。
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