JP6308998B2 - 触媒ナノワイヤを含む触媒およびそれらの使用 - Google Patents
触媒ナノワイヤを含む触媒およびそれらの使用 Download PDFInfo
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- JP6308998B2 JP6308998B2 JP2015514205A JP2015514205A JP6308998B2 JP 6308998 B2 JP6308998 B2 JP 6308998B2 JP 2015514205 A JP2015514205 A JP 2015514205A JP 2015514205 A JP2015514205 A JP 2015514205A JP 6308998 B2 JP6308998 B2 JP 6308998B2
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- catalyst
- catalyst material
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- catalytic
- methane
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 338
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- 239000011148 porous material Substances 0.000 claims description 57
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 claims description 53
- 239000008188 pellet Substances 0.000 claims description 52
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- Dispersion Chemistry (AREA)
Description
例えばOCM反応における不均一触媒の使用は、特に商業規模でのいくつかの課題を提起する。商業的触媒プロセスは、高い時間当たりのガス空間速度での反応(例えば、炭化水素)原材料の高い転換率を達成できなければならない。しかし、不均一触媒の固定ベッドを使用する場合、触媒ベッド両端での圧力低下は、商業運転で要求される高いガス空間速度のもとでの運転を妨害する。さらに、OCMなどの多くの商業的に重要な触媒反応は発熱的であり、触媒ベッド内での発熱(すなわち、ホットスポット)を制御するのが困難である可能性がある。最後に、商業的に重要な多くの不均一触媒は高価でかつ/または希少な金属を含み、したがって、所与のプロセスのために使用される触媒の量を低減するための方法が一般に望まれる。
他の実施形態では、本発明は、本明細書で説明する触媒材料または反応器であって、その触媒材料が、5keVでの明視野モードでTEMにより測定して、1の有効長と実際長の比および10超のアスペクト比を有する無機触媒ナノワイヤを含む触媒材料または反応器のいずれかを対象とする。
本発明は、例えば、以下を提供する。
(項目1)
複数の触媒ナノワイヤを希釈剤と組み合わせて含む触媒材料であって、該希釈剤が、アルカリ土類金属化合物、炭化ケイ素、コージライト、B 2 O 3 、In 2 O 3 、SrAl 2 O 4 、B 4 SrO 7 またはその組合せを含み、該アルカリ土類金属化合物が、MgO、CaO、MgAl 2 O 4 またはアルミン酸カルシウムではない触媒材料。
(項目2)
前記アルカリ土類金属化合物が、MgCO 3 、MgSO 4 、Mg 3 (PO 4 ) 2 、CaCO 3 、CaSO 4 、Ca 3 (PO 4 ) 2 、CaAl 2 O 4 、SrO、SrCO 3 、SrSO 4 、Sr 3 (PO 4 ) 2 、SrAl 2 O 4 、BaO、BaCO 3 、BaSO 4 、Ba 3 (PO 4 ) 2 、BaAl 2 O 4 またはその組合せである、項目1に記載の触媒材料。
(項目3)
前記アルカリ土類金属化合物が、SrO、MgCO 3 、CaCO 3 、SrCO 3 またはその組合せである、項目1に記載の触媒材料。
(項目4)
前記触媒材料が成形集合体を含む、項目1〜3のいずれか一項に記載の触媒材料。
(項目5)
前記成形集合体が押し出し物を含む、項目4に記載の触媒材料。
(項目6)
前記成形集合体が、圧縮またはキャスト粒子を含む、項目4に記載の触媒材料。
(項目7)
前記成形集合体がモノリスを含む、項目4に記載の触媒材料。
(項目8)
前記触媒材料が円筒、ロッド、星形、リブ状、三葉、ディスク、中空、ドーナツ、リング状、ペレット、管、球形、ハニカム、コップ、ボウルおよび不規則形状から選択される形状である、項目1〜7のいずれか一項に記載の触媒材料。
(項目9)
前記触媒材料がモノリス、発泡体、箔、細目網またはハニカム構造上に配置され、その中に含浸され、またはその組合せである、項目1〜7のいずれか一項に記載の触媒材料。
(項目10)
前記触媒材料が1〜50m 2 /gの範囲の表面積を含む、項目1〜9のいずれか一項に記載の触媒材料。
(項目11)
前記触媒材料が20〜90%の範囲の細孔容積率を含む、項目1〜10のいずれか一項に記載の触媒材料。
(項目12)
触媒ナノワイヤと全希釈剤および支持体の重量比が95:5〜5:95の範囲である、項目1〜11のいずれか一項に記載の触媒材料。
(項目13)
前記希釈剤が、前記触媒ナノワイヤの触媒活性を促進するドーパントを含む、項目1〜12のいずれか一項に記載の触媒材料。
(項目14)
前記ドーパントが、OCM反応における前記触媒ナノワイヤの触媒活性を促進する、項目13に記載の触媒材料。
(項目15)
複数の触媒ナノワイヤおよび犠牲的結合剤を含む触媒材料。
(項目16)
圧縮ペレットまたは押し出し物の形態の触媒材料であって、該触媒材料は複数の触媒ナノワイヤを含み、結合剤材料を実質的に含まない触媒材料。
(項目17)
前記触媒材料が組み合わせて合計で1w/w%未満の結合剤および希釈剤を含む、項目16に記載の触媒材料。
(項目18)
前記触媒材料は結合剤も希釈剤も含まない、項目16に記載の触媒材料。
(項目19)
活性触媒およびナノワイヤ結合剤を含む触媒材料。
(項目20)
前記活性触媒がバルク触媒である、項目19に記載の触媒材料。
(項目21)
前記活性触媒が触媒ナノワイヤである、項目19に記載の触媒材料。
(項目22)
前記活性触媒がゼオライト触媒である、項目19に記載の触媒材料。
(項目23)
成形集合体の形態の触媒材料であって、該触媒材料が複数の触媒ナノワイヤおよび希釈剤を含む触媒材料。
(項目24)
前記成形集合体が、押し出し物、圧縮粒子、キャスト粒子またはモノリスである、項目23に記載の触媒材料。
(項目25)
前記触媒材料が20nm超の直径の細孔を含む、項目23または24のいずれか一項に記載の触媒材料。
(項目26)
前記触媒材料の形状が、円筒、ロッド、星形、リブ状、三葉、ディスク、中空、ドーナツ、リング状、ペレット、管、球形、ハニカム、コップ、ボウルおよび不規則形状から選択される、項目23〜25のいずれか一項に記載の触媒材料。
(項目27)
前記押し出し物が内部コアおよび外層を含む、項目23〜26のいずれか一項に記載の触媒材料。
(項目28)
前記触媒ナノワイヤの95%超が前記内部コア中に存在する、項目27に記載の触媒材料。
(項目29)
前記外層が酸素透過性である、項目27または28のいずれか一項に記載の触媒材料。
(項目30)
前記触媒ナノワイヤの95%超が前記外層中に存在する、項目27に記載の触媒材料。
(項目31)
前記希釈剤が、Al 2 O 3 、SiO 2 、TiO 2 、MgO、CaO、SrO、BaO、ZrO 2 、ZnO、LiAlO 2 、MgAl 2 O 4 、MnO、MnO 2 、Mn 3 O 4 、La 2 O 3 、AlPO 4 、SiO 2 /Al 2 O 3 、B 2 O 3 、Ga 2 O 3 、In 2 O 3 、SrAl 2 O 4 、B 4 SrO 7 、CaCO 3 、SrCO 3 、活性炭、シリカゲル、ゼオライト、活性粘土、活性Al 2 O 3 、SiC、珪藻土、アルミノケイ酸塩、アルミン酸カルシウム、アルミン酸バリウム、CeO 2 、硫酸塩、支持体ナノワイヤ、炭化物、炭化ホウ素、炭化ケイ素、窒化物、炭酸塩、炭酸アンモニウム、ケイ酸塩、アルミン酸塩またはその組合せを含む、項目23〜30のいずれか一項に記載の触媒材料。
(項目32)
前記触媒材料が1〜50m 2 /gの範囲の表面積を含む、項目23〜31のいずれか一項に記載の触媒材料。
(項目33)
前記触媒材料が20〜90%の範囲の細孔容積率を含む、項目23〜32のいずれか一項に記載の触媒材料。
(項目34)
触媒ナノワイヤと全希釈剤および支持体の重量比が95:5〜5:95の範囲である、項目23〜33のいずれか一項に記載の触媒材料。
(項目35)
前記希釈剤が、前記触媒ナノワイヤの触媒活性を促進するドーパントを含む、項目23〜34のいずれか一項に記載の触媒材料。
(項目36)
前記ドーパントが、OCM反応における前記触媒ナノワイヤの触媒活性を促進する、項目35に記載の触媒材料。
(項目37)
構造化支持体上またはその中に支持された複数の触媒ナノワイヤを含む触媒材料。
(項目38)
前記構造化支持体が、発泡体、箔、細目網またはハニカム構造を含む、項目37に記載の触媒材料。
(項目39)
前記構造化支持体が炭化ケイ素またはアルミナを含む、項目37または38のいずれか一項に記載の触媒材料。
(項目40)
前記構造化支持体が、金属発泡体、セラミック発泡体、炭化ケイ素発泡体、アルミナ発泡体、波形金属箔または押し出し型セラミックハニカムを含む、項目37〜39のいずれか一項に記載の触媒材料。
(項目41)
前記触媒ナノワイヤが前記構造化支持体上に配置されている、項目37〜40のいずれか一項に記載の触媒材料。
(項目42)
前記触媒ナノワイヤが、1〜10ミクロンの範囲の厚さを有する構造化支持体上に層を形成する、項目41に記載の触媒材料。
(項目43)
前記触媒ナノワイヤが、前記構造化支持体中に含浸されている、項目37〜40のいずれか一項に記載の触媒材料。
(項目44)
前記構造化支持体がモノリスである、項目37〜43のいずれか一項に記載の触媒材料。
(項目45)
前記モノリスがガス透過性の壁を含む、項目44に記載の触媒材料。
(項目46)
前記ガス透過性の壁が酸素透過性である、項目45に記載の触媒材料。
(項目47)
前記モノリスが複数のフローチャネルを含む、項目45または46のいずれか一項に記載の触媒材料。
(項目48)
前記モノリスが活性フローチャネルおよび不活性フローチャネルを含み、前記活性フローチャネルが触媒ナノワイヤを含み、前記不活性フローチャネルが触媒ナノワイヤを実質的に含まない、項目47に記載の触媒材料。
(項目49)
前記フローチャネルの5〜75%が不活性フローチャネルである、項目48に記載の触媒材料。
(項目50)
前記フローチャネルが、ガス流を、交互になっている活性および不活性フローチャネルを通して導くように構成されている、項目48または49のいずれか一項に記載の触媒材料。
(項目51)
前記構造化支持体が、前記触媒ナノワイヤの触媒活性を促進するドーパントを含む、項目37〜50のいずれか一項に記載の触媒材料。
(項目52)
前記ドーパントが、OCM反応における前記触媒ナノワイヤの触媒活性を促進する、項目51に記載の触媒材料。
(項目53)
第1および第2の触媒を含む触媒材料であって、前記第1および第2の触媒が、同じ条件下での同じ反応において異なる触媒活性を有する触媒材料。
(項目54)
前記第1の触媒がナノワイヤ触媒である、項目53に記載の触媒材料。
(項目55)
前記第2の触媒がバルク触媒である、項目53または54のいずれか一項に記載の触媒材料。
(項目56)
前記第1および第2の触媒のそれぞれがナノワイヤ触媒である、項目53に記載の触媒材料。
(項目57)
前記第1および第2の触媒のそれぞれがバルク触媒である、項目53に記載の触媒材料。
(項目58)
前記第2の触媒が、同じ条件下で前記第1の触媒より低い触媒活性を有する、項目53〜57のいずれか一項に記載の触媒材料。
(項目59)
前記第2の触媒の触媒活性が温度の上昇に伴って増大する、項目57に記載の触媒材料。
(項目60)
前記反応がOCMである、項目53〜59のいずれか一項に記載の触媒材料。
(項目61)
前記触媒材料が750℃または750℃より低い温度でのメタンの酸化カップリングにおける触媒材料として使用される場合に、25%超の1回通過でのメタン転換率を有する触媒材料。
(項目62)
前記触媒材料が反応器と接触している、触媒ナノワイヤを含む触媒材料。
(項目63)
前記反応器が、OCMを実施するために使用される、項目62に記載の触媒材料。
(項目64)
前記触媒材料が炭化ケイ素を含む、項目62または63のいずれか一項に記載の触媒材料。
(項目65)
前記反応器が固定ベッド反応器である、項目62〜64のいずれか一項に記載の触媒材料。
(項目66)
前記反応器が少なくとも1インチの内径を含む、項目62〜65のいずれか一項に記載の触媒材料。
(項目67)
少なくとも1つのO 2 −OCM触媒および少なくとも1つのCO 2 −OCM触媒を含む触媒材料。
(項目68)
前記O 2 −OCM触媒または前記CO 2 −OCM触媒の少なくとも1つが触媒ナノワイヤである、項目67に記載の触媒材料。
(項目69)
少なくとも1つのO 2 −OCM触媒および少なくとも1つのCO 2 −ODH触媒を含む触媒材料。
(項目70)
前記O 2 −OCM触媒または前記CO 2 −ODH触媒の少なくとも1つが触媒ナノワイヤである、項目69に記載の触媒材料。
(項目71)
前記触媒材料が約35%〜約70%の容積空隙率を含む、項目1〜70のいずれか一項に記載の触媒材料。
(項目72)
前記触媒材料が約45%〜約65%の容積空隙率を含む、項目71に記載の触媒材料。
(項目73)
前記触媒材料が約1mm〜約20mmの範囲の少なくとも1つの寸法の断面寸法を有する触媒粒子を含む、項目1〜72のいずれか一項に記載の触媒材料。
(項目74)
前記断面寸法が、約2mm〜約10mmの範囲である、項目73に記載の触媒材料。
(項目75)
前記触媒材料が約0.1mm −1 〜約10mm −1 の範囲の表面積と容積の比を有する触媒粒子を含む、項目1〜74のいずれか一項に記載の触媒材料。
(項目76)
前記触媒材料が約0.1mm −1 〜約5mm −1 の範囲の表面積と容積の比を有する触媒粒子を含む、項目75に記載の触媒材料。
(項目77)
前記触媒材料が約1N/mm 2 超の破壊強度を含む、項目1〜76のいずれか一項に記載の触媒材料。
(項目78)
前記触媒材料が約10N/mm 2 超の破壊強度を含む、項目77に記載の触媒材料。
(項目79)
前記触媒材料が約10%〜約80%の間の多孔率を含む、項目1〜78のいずれか一項に記載の触媒材料。
(項目80)
前記多孔率が約40%〜約60%の間である、項目79に記載の触媒材料。
(項目81)
触媒形態エンベロープの表面積と触媒形態エンベロープの容積の比が、約0.5mm −1 〜約4mm −1 の範囲である、項目1〜80のいずれか一項に記載の触媒材料。
(項目82)
前記触媒材料が均一に分散された活性触媒を含む、項目1〜81のいずれか一項に記載の触媒材料。
(項目83)
前記触媒材料が約1m 2 /g〜約50m 2 /gの範囲の表面積を含む、項目1〜82のいずれか一項に記載の触媒材料。
(項目84)
触媒ベッドを含む反応器であって、該触媒ベッドが入口端、出口端ならびに活性触媒および希釈剤を含む触媒材料を含み、該触媒ベッドが該活性触媒の濃度勾配を含み、前記活性触媒の濃度が、該出口端より該入口端において高い反応器。
(項目85)
前記活性触媒がOCM活性触媒である、項目84に記載の反応器。
(項目86)
前記反応器をメタンの酸化カップリングのために使用する場合、前記濃度勾配が、前記入口端から前記出口端への温度変化が200℃を超えないように選択される、項目84または85のいずれか一項に記載の反応器。
(項目87)
前記触媒材料が無機触媒性多結晶ナノワイヤを含み、該ナノワイヤが、5keVでの明視野モードでTEMにより測定して、1未満の有効長と実際長の比および10超のアスペクト比を有し、該ナノワイヤが、1族〜7族、ランタニド、アクチニドまたはその組合せのいずれかからの1つまたは複数の元素を含む、項目1〜86のいずれか一項に記載の触媒材料または反応器。
(項目88)
触媒材料を調製するための方法であって、該方法は複数の触媒ナノワイヤを犠牲的結合剤と混合するステップと、該犠牲的結合剤を除去して、結合剤材料を実質的に含まず、該犠牲的結合剤なしで調製された触媒材料と比べて増大した微小細孔を有する触媒材料を得るステップとを含む方法。
(項目89)
メタンの酸化カップリングのための方法であって、該方法は触媒材料の存在下でメタンを1つまたは複数のC2炭化水素へ転換させるステップを含み、該触媒材料が少なくとも1つのO 2 −OCM触媒および少なくとも1つのCO 2 −OCM触媒を含む方法。
(項目90)
前記O 2 −OCM触媒または前記CO 2 −OCM触媒の少なくとも1つが、触媒ナノワイヤである、項目89に記載の方法。
(項目91)
前記触媒材料が、O 2 −OCM触媒とCO 2 −OCM触媒が交互になっている層のベッドを含む、項目89または90のいずれか一項に記載の方法。
(項目92)
前記触媒材料が、O 2 −OCM触媒とCO 2 −OCM触媒の均一混合物を含む、項目89または90のいずれか一項に記載の方法。
(項目93)
エチレンの調製のための方法であって、触媒材料の存在下でメタンをエチレンへ転換させるステップを含み、前記触媒材料が少なくとも1つのO 2 −OCM触媒および少なくとも1つのCO 2 −ODH触媒を含む方法。
(項目94)
前記O 2 −OCM触媒または前記CO 2 −OCM触媒の少なくとも1つが触媒ナノワイヤである、項目93に記載の方法。
(項目95)
メタンの酸化カップリングのための方法であって、項目1〜87のいずれか一項に記載の触媒材料または反応器を、メタンと酸素を含む混合物と接触させるステップを含む方法。
(項目96)
エタンまたはエチレンの調製のための方法であって、項目1〜87のいずれか一項に記載の触媒材料または反応器を、メタンと酸素を含む混合物と接触させるステップを含む方法。
(項目97)
エチレンの川下製品の調製のための方法であって、該方法はエチレンをオリゴマー化するステップを含み、該エチレンが、項目1〜87のいずれかに記載の触媒材料または反応器をメタンと酸素を含む混合物と接触させるステップを含む方法によって調製されている方法。
定義
1.触媒
2.触媒配合物
A.ナノワイヤ配合物
3.触媒形態
上記実施形態は、局部O2濃度を低下させ、局部温度を上昇させ、かつ/またはこれらのラジカルの比が不都合になってきた場合に中間ラジカルの濃度の急な勾配を生み出すことによって、活性形態のコア内の局部環境を促進し、OCM反応の選択率の向上をもたらすと考えられる。形成された粒子間を流れるガスとその粒子のコア内にある活性触媒との間の境界層上の拡散抵抗調整の場合での特定の望ましい効果には、
1− 粒子内の温度勾配の調整(一般に不活性コーティングがない場合より大きい);
2− 非触媒活性ゾーンにおける酸素勾配の発生(O2は半化学量論的種(specie)であるので、燃料と酸素の間の微分的な浸透なしで、粒子内で大きいO2濃度勾配が形成される可能性がある);および
が含まれる。
4.触媒材料の調製
触媒反応
1.メタンの酸化カップリング(OCM)
エチレンへのメタンの選択的な触媒的酸化カップリング(すなわち、OCM反応)は以下の反応(1)で示される:
2CH4+O2→CH2CH2+2H2O (1)
不均一触媒の表面上でのOCM反応は、図式的には図2に表される。この反応は発熱的(反応熱−67kcal/mole)であり、通常、非常に高温(>700℃)で起こる。この反応の間、メタン(CH4)はまず酸化的にカップリングされてエタン(C2H6)となり、続いてこのエタン(C2H6)が酸化的に脱水素化されてエチレン(C2H4)となると考えられる。反応で用いられる高温のため、エタンは、表面発生メチル(CH3)ラジカルの気相中のカップリングによって主に生成することが示唆されている。CH4を活性化してCH3ラジカルを生成するためには、反応性金属酸化物(酸素型イオン)が明らかに必要である。C2H4およびC2H6の収率は、気相中およびある程度の触媒表面でのさらなる反応によって限定される。メタンの酸化の際に起こる、可能性のある若干の反応は反応(2)〜(8)として以下に示す:
CH4→CH3ラジカル (2)
CH3ラジカル→C2H6 (3)
CH3ラジカル+2.5O2→CO2+1.5H2O (4)
C2H6→C2H4+H2 (5)
C2H6+0.5O2→C2H4+H2O (6)
C2H4+3O2→2CO2+2H2O (7)
CH3ラジカル+CxHy+O2→高級HCの酸化/CO2+H2O (8)
2.酸化的脱水素化
一実施形態では、触媒材料は、炭化水素(例えば、アルカン、アルケンおよびアルキン)の酸化的脱水素化(ODH)を触媒作用するのに有用である。例えば、一実施形態では、これらの触媒材料は、エタンまたはプロパンをそれぞれエチレンまたはプロピレンへ転換させるODH反応の触媒反応に有用である。反応スキーム(9)は、炭化水素の酸化的脱水素化を表す:
CxHy+1/2O2→CxHy−2+H2O (9)
本開示の1つの実施形態は、エタンの酸化的脱水素化の触媒作用をするために代替の酸素源(例えば、CO2、H2O、SO2、SO3またはその組合せ)を使用することができる触媒材料を提供することを対象とする。例えば、そのODH反応は以下の反応(10):
CO2+CxHy→CxHy−2+CO+H2O (10)
に従って進行させることができる。
3.メタンの二酸化炭素リフォーミング
CO2+CH4→2CO+2H2 (11)
に例示される。
2CO→C+CO2 (12)
CH4→C+2H2 (13)
4.フィッシャー・トロプシュ合成
CO+2H2→(1/n)(CnH2n)+H2O (14)
5.COの酸化
一酸化炭素(CO)は有毒ガスであり、ヘモグロビンを、窒息をもたらすカルボキシヘモグロビンへ転換させることができる。COの危険レベルは、反応スキーム15に示すようなCOのCO2への酸化によって軽減させることができる:
CO+1/2O2→CO2 (15)
6.炭化水素の燃焼
7.触媒特性の評価
8.川下製品
支持されたMnWO4ナノワイヤ触媒の調製
支持されたMnWO4ナノワイヤ触媒は、以下の一般的プロトコルを用いて調製する。MnWO4ナノワイヤは、米国特許公開第2012/0041246号に記載されている方法を用いて調製する。タングステン酸マンガンナノワイヤ、支持体および水を、室温で6hスラリー化する。タングステン酸マンガンと支持体の比は2〜10wt%の範囲である。混合物を65℃オーブン中で乾燥し、次いでマッフルオーブンにおいて空気中で焼成し、室温で加熱炉に載せ、5℃/minの速度で400℃へ昇温し、2h保持し、5℃/minの速度で850℃へ昇温し、8h保持し、室温に冷却する。以下は、使用できる例示的な支持体のリストである:SiO2、Al2O3、SiO2−Al2O3、ZrO2、TiO2、HfO2、シリカ−リン酸アルミニウムおよびリン酸アルミニウム。
(実施例2)
コージライトハニカムセラミック支持されたNd2O3ナノワイヤを含む触媒材料の調製
(実施例3)
炭化ケイ素セラミック発泡体支持されたNd2O3ナノワイヤを含む触媒材料の調製
(実施例4)
炭化ケイ素およびNd2O3ナノワイヤを含む触媒材料の調製
(実施例5)
La2O3ナノワイヤペレットの調製
(実施例6)
CaOをブレンドされたLa2O3ナノワイヤのペレットの調製
(実施例7)
La2O3ナノワイヤ押し出し物の調製
(実施例8)
CaOをブレンドされたLa2O3ナノワイヤの押し出し物の調製
(実施例9)
CaOをブレンドされたLa2O3ナノワイヤの押し出し物の調製
(実施例10)
SiCをブレンドされたLa2O3ナノワイヤのペレットの調製
(実施例11)
種々の成形集合体の評価
Claims (29)
- 成形集合体の形態のメタンの酸化カップリングのための触媒材料であって、該触媒材料が複数の触媒ナノワイヤおよび希釈剤を含み、該成形集合体が、内部コアおよび外層を含む押し出し物である、触媒材料。
- 前記触媒材料が20nm超の直径の細孔を含む、請求項1に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒材料の形状が、円筒、ロッド、星形、リブ状、三葉、ディスク、中空、ドーナツ、リング状、ペレット、管、球形、ハニカム、コップ、ボウルおよび不規則形状から選択される、請求項1〜2のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒ナノワイヤの95%超が前記内部コア中に存在する、請求項1〜3のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記外層が酸素透過性である、請求項1〜4のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒ナノワイヤの95%超が前記外層中に存在する、請求項1〜5のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記希釈剤が、Al2O3、SiO2、TiO2、MgO、CaO、SrO、BaO、ZrO2、ZnO、LiAlO2、MgAl2O4、MnO、MnO2、Mn3O4、La2O3、AlPO4、SiO2/Al2O3、B2O3、Ga2O3、In2O3、SrAl2O4、B4SrO7、CaCO3、SrCO3、活性炭、シリカゲル、ゼオライト、活性粘土、活性Al2O3、SiC、珪藻土、アルミノケイ酸塩、アルミン酸カルシウム、アルミン酸バリウム、CeO2、硫酸塩、支持体ナノワイヤ、炭化物、炭化ホウ素、炭化ケイ素、窒化物、炭酸塩、炭酸アンモニウム、ケイ酸塩、アルミン酸塩またはその組合せを含む、請求項1〜6のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒材料が1〜50m2/gの範囲の表面積を含む、請求項1〜7のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒材料が20〜90%の範囲の細孔容積率を含む、請求項1〜8のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 触媒ナノワイヤと全希釈剤および支持体の重量比が95:5〜5:95の範囲である、請求項1〜9のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記希釈剤が、前記触媒ナノワイヤの触媒活性を促進するドーパントを含む、請求項1〜10のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記ドーパントが、OCM反応における前記触媒ナノワイヤの触媒活性を促進する、請求項11に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒材料が約35%〜約70%の容積空隙率を含む、請求項1〜12のいずれか一項に記載のメタンの酸化カップリングのための触媒材料。
- 前記触媒材料が約45%〜約65%の容積空隙率を含む、請求項13に記載の触媒材料。
- 前記触媒材料が約1mm〜約20mmの範囲の少なくとも1つの寸法の断面寸法を有する触媒粒子を含む、請求項1〜13のいずれか一項に記載の触媒材料。
- 前記断面寸法が、約2mm〜約10mmの間である、請求項15に記載の触媒材料。
- 前記触媒材料が約0.1mm−1〜約10mm−1の間の表面積と容積の比を有する触媒粒子を含む、請求項1〜16のいずれか一項に記載の触媒材料。
- 前記触媒材料が約0.1mm−1〜約5mm−1の範囲の表面積と容積の比を有する触媒粒子を含む、請求項17に記載の触媒材料。
- 前記触媒材料が1N/mm2超の破壊強度を含む、請求項1〜18のいずれか一項に記載の触媒材料。
- 前記触媒材料が10N/mm2超の破壊強度を含む、請求項19に記載の触媒材料。
- 前記触媒材料が約10%〜約80%の間の多孔率を含む、請求項1〜20のいずれか一項に記載の触媒材料。
- 前記多孔率が約40%〜約60%の間である、請求項21に記載の触媒材料。
- 触媒形態エンベロープの表面積と触媒形態エンベロープの容積の比が、約0.5mm−1〜約4mm−1の範囲である、請求項1〜22のいずれか一項に記載の触媒材料。
- 前記触媒ナノワイヤが前記触媒材料中に均一に分散されている、請求項1〜23のいずれか一項に記載の触媒材料。
- 前記触媒材料が約1m2/g〜約50m2/gの範囲の表面積を含む、請求項1〜24のいずれか一項に記載の触媒材料。
- 前記触媒材料が無機触媒性多結晶ナノワイヤを含み、該ナノワイヤが、5keVでの明視野モードでTEMにより測定して、1未満の有効長と実際長の比および10超のアスペクト比を有し、該ナノワイヤが、1族〜7族、ランタニド、アクチニドまたはその組合せのいずれかからの1つまたは複数の元素を含む、請求項1〜25のいずれか一項に記載の触媒材料。
- メタンの酸化カップリングのための方法であって、請求項1〜26のいずれか一項に記載の触媒材料を、メタンと酸素を含む混合物と接触させるステップを含む方法。
- エタンまたはエチレンの調製のための方法であって、請求項1〜26のいずれか一項に記載の触媒材料を、メタンと酸素を含む混合物と接触させるステップを含む方法。
- エチレンの川下製品の調製のための方法であって、該方法はエチレンをオリゴマー化するステップを含み、該エチレンが、請求項1〜26のいずれかに記載の触媒材料をメタンと酸素を含む混合物と接触させるステップを含む方法によって調製されている方法。
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
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US10974226B2 (en) | 2018-09-24 | 2021-04-13 | Sabic Global Technologies B.V. | Catalytic process for oxidative coupling of methane |
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AU2013266189B2 (en) | 2018-01-04 |
US11370724B2 (en) | 2022-06-28 |
CA3125016A1 (en) | 2013-11-28 |
AU2013266189A1 (en) | 2014-12-11 |
EP2855011A2 (en) | 2015-04-08 |
CA2874043C (en) | 2021-09-14 |
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HK1209079A1 (en) | 2016-03-24 |
US20140121433A1 (en) | 2014-05-01 |
WO2013177461A3 (en) | 2014-01-16 |
CA2874043A1 (en) | 2013-11-28 |
US20200024214A1 (en) | 2020-01-23 |
WO2013177461A2 (en) | 2013-11-28 |
JP2015522407A (ja) | 2015-08-06 |
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