JP5122178B2 - 水素化/脱水素化反応用担持触媒、その製造方法、およびその触媒を用いた水素貯蔵/供給方法 - Google Patents
水素化/脱水素化反応用担持触媒、その製造方法、およびその触媒を用いた水素貯蔵/供給方法 Download PDFInfo
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Description
図1に示す水素化および脱水素化反応装置において、後述の各実施例および比較例の試料を用いて、シクロヘキサンあるいはメチルシクロヘキサンの脱水素化反応を行った。反応条件としては、設定温度320℃、反応圧力0.1MPaG、触媒層体積4.3ml、原料投入速度0.15ml/min、液空間速度2.0h−1、および水素添加量10ml/min(水素/oil比0.3mol/1mol)に設定した。また、水素発生速度とシクロヘキサンの転化率は、ガスクロマトグラフィーにより分析することにより求めた。シクロヘキサンの脱水素化反応を行った際の、水素発生速度、シクロヘキサン転化率、およびベンゼン選択率を表1に示した。また、メチルシクロヘキサンの脱水素化反応を行った際の、水素発生速度、メチルシクロヘキサン転化率、およびトルエン選択率を表2に示した。さらに、シクロヘキサンの脱水素化反応を行った際の、反応速度の時間変化を表3に示した。
シクロヘキサン(メチルシクロヘキサン)転化率(%)=(生成したベンゼン(トルエン)のモル数/原料のシクロヘキサン(メチルシクロヘキサン)のモル数)×100
ベンゼン(トルエン)選択率(%)=(生成したベンゼン(トルエン)のモル数/原料のシクロヘキサン(メチルシクロヘキサン)のモル数)×100
水素生成速度(mL/min)=毎分あたりの生成した水素の容量
水素生成活性(mL/min/g)=白金1gあたりの毎分あたりの生成した水素の容量
白金18mgを含む塩化白金酸H2PtCl6水溶液を、モリブデンカーバイドへ噴霧した後、窒素ガス雰囲気下350℃で3時間の焼成を行った。その後、窒素ガスで希釈した10%水素雰囲気下で室温から350℃まで段階的に昇温して調製して、0.5%白金担持モリブデンカーバイド(Pt/Mo2C)触媒を作製した。
担体として、活性炭、メソ多孔質シリケート(FSM−16)、シリカおよびアルミナをそれぞれ用いて、モリブデン酸アンモニウムを含む溶液を担体に塗布した後、空気雰囲気下350℃で加熱した。そして酸化モリブデンを担持した活性炭、メソ多孔質シリケート、シリカおよびアルミナを、体積比にて、メタン(あるいはブタン):水素=1:10の混合ガス雰囲気下にて350〜500℃で段階的に5時間の加熱反応を行うことにより、酸化モリブデンをモリブデンカーバイドに変換した。
白金18mgを含む塩化白金酸H2PtCl6水溶液を、担体である活性炭に噴霧した後、窒素ガス下350℃で3時間の焼成を行った。その後、窒素ガスで希釈した10%水素雰囲気下において、室温〜350℃まで段階的に昇温して、0.5%白金担持活性炭(Pt/AC)触媒を調製した(比較例1)。
縦40mm、横40mmおよび厚さ5mmの形状を有するアルミニウム板を、温度20℃の環境下で、4wt%シュウ酸溶液を電解質溶液として用いて、0.5A/dm2Nの電流密度で7時間陽極酸化を行い、50ミクロンの厚さの陽極酸化皮膜を得た。その後20℃に加熱した4wt%シュウ酸溶液に5分間浸漬することで拡孔処理を行った。
また、白金18mgを含む塩化白金酸H2PtCl6水溶液を、多孔質アルマイト担体の多孔質アルミナ面に噴霧した後、空気気流下350〜500℃で3時間焼成を行った。その後、窒素で希釈した10%水素雰囲気下において、室温〜350℃まで段階的に昇温することにより、多孔質アルマイトの表面積1m2あたりに白金3gを担持している白金担持アルマイト触媒(3g/m2 Pt/Al2O3/Al)を調製した(比較例2)。
Claims (9)
- 担体の表面の一部または全部は、モリブデンカーバイド、タングステンカーバイドのいずれか一方の金属カーバイドと白金とにより覆われており、前記担体は、微細孔を有するアルミナを反応面に有した多孔質体であって、当該反応面の逆側の面に、アルミニウム、アルミニウム合金、アルミニウムを含む鉄合金、または表面にアルミニウムを張り合わせた耐熱合金のいずれか一つの金属が、上記アルミナを保持していることを特徴とする水素化および脱水素化反応用担持触媒。
- 前記反応面側にあるアルミニウムを、陽極酸化により微細孔を有するアルミナに転化させたものであることを特徴とする請求項1に記載の水素化および脱水素化反応用担持触媒。
- 前記微細孔を有するアルミナが、前記陽極酸化皮膜の形成の後に焼成処理によって形成されたものであることを特徴とする請求項2に記載の水素化および脱水素化反応用担持触媒。
- 前記微細孔を有するアルミナが、前記陽極酸化皮膜の形成の後に前記焼成処理の前に拡孔処理を経て形成されたものであることを特徴とする請求項3に記載の水素化および脱水素化反応用担持触媒。
- 前記反応面側にあるアルミニウムが異種金属とのクラッド材を形成していることを特徴とする請求項1から4のいずれか1項記載の水素化および脱水素化反応用担持触媒。
- 前記異種金属が鉄またはステンレス鋼であることを特徴とする請求項5に記載の水素化および脱水素化反応用担持触媒。
- ベンゼンもしくはトルエンの水素化反応、またはシクロヘキサンもしくはメチルシクロヘキサンの脱水素化反応である請求項1から6のいずれか1項記載の水素化および脱水素化反応用担持触媒。
- 担体の表面の一部または全部は、モリブデンカーバイド、タングステンカーバイドのいずれか一方と白金とにより覆われており、前記担体は、微細孔を有するアルミナを反応面に有した多孔質体であって、当該反応面の逆側の面に、アルミニウム、アルミニウム合金、アルミニウムを含む鉄合金、または表面にアルミニウムを張り合わせた耐熱合金のいずれか一つの金属が、上記アルミナを保持した触媒を用いて、芳香族化合物への水素化反応または当該水素化誘導体の脱水素化反応を行うことを特徴とする水素貯蔵および水素供給方法。
- ベンゼンもしくはトルエンの水素化反応、またはシクロヘキサンもしくはメチルシクロヘキサンの脱水素化反応を行うことを特徴とする請求項8記載の水素貯蔵および水素供給方法。
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JP2007118578A JP5122178B2 (ja) | 2007-04-27 | 2007-04-27 | 水素化/脱水素化反応用担持触媒、その製造方法、およびその触媒を用いた水素貯蔵/供給方法 |
PCT/JP2008/057413 WO2008136264A1 (ja) | 2007-04-27 | 2008-04-16 | 水素化/脱水素化反応用担持触媒、その製造方法、およびその触媒を用いた水素貯蔵/供給方法 |
CN200880022491A CN101801841A (zh) | 2007-04-27 | 2008-04-16 | 氢化/脱氢化反应用载体催化剂、其制备方法以及使用该催化剂的氢储存/供给方法 |
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JP5489509B2 (ja) * | 2009-03-31 | 2014-05-14 | 日立エーアイシー株式会社 | 水素触媒部材 |
JP5489508B2 (ja) * | 2009-03-31 | 2014-05-14 | 日立エーアイシー株式会社 | 水素触媒部材 |
JP5620077B2 (ja) * | 2009-06-11 | 2014-11-05 | 日立エーアイシー株式会社 | 水素触媒部材 |
EP2305376A1 (en) * | 2009-09-23 | 2011-04-06 | Lonza Ltd. | Process and catalyst for the catalytic hydrogenation of aromatic and heteroaromatic nitro compounds |
JP2013518710A (ja) * | 2010-02-05 | 2013-05-23 | ビーエーエスエフ ソシエタス・ヨーロピア | 触媒の製造方法及び触媒 |
JP5369126B2 (ja) * | 2010-04-28 | 2013-12-18 | 日本精線株式会社 | 水素化反応/脱水素化反応用のワイヤー触媒成形品 |
KR101688524B1 (ko) | 2010-07-30 | 2016-12-22 | 삼성전자주식회사 | 연료전지용 전극촉매, 이 전극촉매를 포함하는 막 전극 접합체와 연료전지, 및 연료전지용 전극촉매의 제조방법 |
WO2012106349A2 (en) * | 2011-01-31 | 2012-08-09 | The Regents Of The University Of Michigan | High activity early transition metal carbide- and nitride-based catalysts |
JP6269297B2 (ja) * | 2014-04-25 | 2018-01-31 | トヨタ自動車株式会社 | ピストン頂面皮膜方法 |
CN104307547B (zh) * | 2014-11-03 | 2017-02-15 | 太仓派欧技术咨询服务有限公司 | 一种甲烷二氧化碳催化重整反应中的Pt‑ZrO2/WC催化剂 |
CN104307546A (zh) * | 2014-11-03 | 2015-01-28 | 太仓派欧技术咨询服务有限公司 | 一种Pt族金属点缀活性点的过渡金属催化剂 |
KR102098066B1 (ko) * | 2018-04-24 | 2020-04-07 | 울산과학기술원 | 고활성 전극 촉매의 제조방법 및 그를 이용하여 제조된 고활성 전극 촉매 |
CN111054410B (zh) * | 2018-10-16 | 2023-04-07 | 中国石油化工股份有限公司 | 液相脱氢催化剂、制备及用途 |
CN110124707B (zh) * | 2019-06-06 | 2022-05-31 | 中山大学 | 一种螺旋状超低铂载量Mo2C催化剂及其制备方法和应用 |
CN115485063A (zh) * | 2020-04-23 | 2022-12-16 | 千代田化工建设株式会社 | 蛋壳型载铂氧化铝催化剂、其制备方法及其使用方法 |
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