JP2005515888A - 制御された(111)結晶面の露出を有する触媒 - Google Patents
制御された(111)結晶面の露出を有する触媒 Download PDFInfo
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- JP2005515888A JP2005515888A JP2003563718A JP2003563718A JP2005515888A JP 2005515888 A JP2005515888 A JP 2005515888A JP 2003563718 A JP2003563718 A JP 2003563718A JP 2003563718 A JP2003563718 A JP 2003563718A JP 2005515888 A JP2005515888 A JP 2005515888A
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Abstract
Description
貴金属塩および有機金属の金属イオン封鎖剤の溶液を調製するステップと、
封鎖された貴金属の溶液を還元剤で処理するステップと、
還元した貴金属溶液を触媒担体に含浸させるステップと、
含浸された担体を乾燥するステップと、
乾燥した含浸担体を還元することによって触媒を活性化して、貴金属粒子の表面上で(111)型の結晶相が優勢であるナノメートルサイズの貴金属触媒を得るステップと
を含む。
特に高い触媒活性度に寄与するナノメートルサイズの粒子を生成する。
知られている金属結晶面の露出状態の制御によって、望ましい生成物への触媒反応の選択性を高める。
触媒の望ましい高い活性度を喪失することになる金属粒子の大きな構造への凝集が、金属微結晶の基材表面への強い結合によって防止される。さらに強い結合によって、触媒の使用中に周囲の液体媒体中に活性金属成分が損耗することが実質上防止される。
触媒による改質は、本質的に炭素−水素結合を切断して、炭素−酸素結合および水素−水素結合を形成することであるので、結合の切断および交換に関する規定の反応を行うためには、活性触媒は互いに隣接する活性部位を持つ構造を有するべきである。図1を参照すると、白金(Pt)の結晶面(110)は、結晶表面層上で、各Pt原子が、2個の隣接するPt原子によって取り囲まれているに過ぎない構造を含むことが認められる。結晶面(100)では、各Pt原子は、4個の他のPt原子に隣接する。しかし、結晶面(111)では、各Pt原子は、6個の他のPt原子に隣接する。したがって、結晶面(111)は、メタンまたはその他の炭化水素を改質するために、C−H結合を切断するより多くの活性部位を表面上に提供するであろうことは明らかである。(111)の部位の隣接特性はまた、隣接する水素原子を再結合させて水素分子を生成し、かつ隣接する部位から炭素に加えて酸素を組合せて炭素酸化物分子、主として一酸化炭素を形成する改質反応の効率を改善するであろう。
(111)結晶相の表面を有するPt触媒を調製するために、所望量の塩化白金を水に溶解する。グリコール酸溶液などの相の制御剤溶液と塩化白金溶液とを、金属対薬剤の比が1:0.5から1:10の間であるように混合した。混合した溶液を窒素でパージし、次いで水素で還元する。形成された有機金属錯体、すなわち、グリコール酸白金が含浸によってアルミナなど触媒担体上に堆積される。含浸中、グリコラートの網状組織がPtを保持し、(111)結晶相のパターンを有する分散物を提供する。得られた試料を空気中で乾燥し、水素中で温度100〜400℃で還元することによって活性化した。その結果、Pt(111)結晶相の表面の露出を有する触媒が得られた。最終触媒は、好ましくは0.01から5重量%、より好ましくは0.01から1重量%の間のPtの負荷を有している。
Claims (22)
- 担持された貴金属触媒であって、貴金属は担体材料上の粒子−担体の制御および結合剤を含むマトリックス内に含まれるナノメートルサイズの結晶粒子を含み、前記結晶粒子は貴金属粒子の表面上に(111)型の結晶相を優勢に有することを特徴とする触媒。
- 前記担体は、多孔性担体材料を含むことを特徴とする請求項1に記載の触媒。
- 前記担体は、活性炭、カーボンブラック、フッ素化炭素、アルミナ、ベントナイト、粘土、ケイ藻土、合成および天然ゼオライト、マグネシア、チタニア、ならびに高分子材料からなる群から選択されることを特徴とする請求項1に記載の触媒。
- 前記担体材料は、少なくとも1グラム当たり20平方メートルの表面積を有することを特徴とする請求項1に記載の触媒。
- 前記貴金属粒子表面の結晶相の少なくとも1/2が(111)型の結晶相を含むことを特徴とする請求項1に記載の触媒。
- 前記制御および結合剤は、有機金属の金属イオン封鎖剤を含むことを特徴とする請求項1に記載の触媒。
- 前記金属イオン封鎖剤は、多官能性低分子量カルボン酸および/または分岐した多官能性高分子カルボン酸を含むことを特徴とする請求項6に記載の触媒。
- 前記金属イオン封鎖剤は、グリコール酸を含むことを特徴とする請求項6に記載の触媒。
- 前記ナノメートルサイズの結晶粒子の粒径は、5ナノメートル未満であることを特徴とする請求項1に記載の触媒。
- 前記粒径は、好ましくは2ナノメートル未満であることを特徴とする請求項1に記載の触媒。
- 前記貴金属は、白金、パラジウム、レニウム、ロジウム、ルテニウム、オスミウムおよびイリジウムからなる群から選択されることを特徴とする請求項1に記載の触媒。
- 前記貴金属は、合計触媒重量の0.01%から10%を構成することを特徴とする請求項1に記載の触媒。
- 前記貴金属は、合計触媒重量の0.1から5%を構成することを特徴とする請求項12に記載の触媒。
- 前記結晶粒子は、さらに、鉄、ニッケル、銅およびスズを含む貴金属以外の金属を含むことを特徴とする請求項1に記載の触媒。
- 貴金属粒子の表面上で(111)型の結晶相が優勢で、ナノメートルサイズの結晶粒子を有する、担持された貴金属触媒を調製する方法であって、
貴金属塩および有機金属の金属イオン封鎖剤の溶液を調製すること、
封鎖された貴金属の溶液を還元剤で処理すること、
還元した貴金属溶液を触媒担体に含浸させること、
含浸された担体を乾燥すること、および
乾燥した含浸担体を還元することによって触媒を活性化し、貴金属粒子の表面上で(111)型の結晶相が優勢であるナノメートルサイズの貴金属触媒を得ること
を含むことを特徴とする方法。 - 前記溶液が、グリコール酸を1:0.5から1:10の間の金属対薬剤の比で含む、貴金属および金属イオン封鎖剤の水溶液であることを特徴とする請求項15に記載の方法。
- 前記乾燥した含浸担体は、100から400℃の間の温度で水素化によって還元されることを特徴とする請求項15に記載の方法。
- 前記担持された活性化触媒は、0.01から10重量パーセントの間の貴金属の負荷を有することを特徴とする請求項15に記載の方法。
- 前記担体は、活性炭、カーボンブラック、フッ素化炭素、アルミナ、ベントナイト、粘土、ケイ藻土、合成および天然ゼオライト、マグネシア、チタニア、ならびに高分子材料からなる群から選択されることを特徴とする請求項15に記載の方法。
- 前記封鎖された貴金属溶液を、水素ガスを含む還元剤で処理することを特徴とする請求項15に記載の方法。
- 前記貴金属塩および有機金属の金属イオン封鎖剤の溶液を、水素ガスを含む還元剤で処理することを特徴とする請求項15に記載の方法。
- 改質条件下で請求項1に記載の触媒を用いてナフサを処理することを含む石油ナフサを改質する方法。
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JP2005224722A (ja) * | 2004-02-13 | 2005-08-25 | Toda Kogyo Corp | オートサーマルリフォーミング触媒及びその製造方法、並びに該オートサーマルリフォーミング触媒を用いた水素の製造方法 |
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JP2007090136A (ja) * | 2005-09-27 | 2007-04-12 | Tanaka Kikinzoku Kogyo Kk | 触媒の製造方法 |
JP4686316B2 (ja) * | 2005-09-27 | 2011-05-25 | 田中貴金属工業株式会社 | 触媒の製造方法 |
JP2009515693A (ja) * | 2005-11-14 | 2009-04-16 | アンスティテュ フランセ デュ ペトロール | 還元剤の存在下に異方性金属ナノ粒子をベースとする触媒の製造方法 |
JP2007239054A (ja) * | 2006-03-09 | 2007-09-20 | Osaka Univ | 四面体パラジウム微粒子、および金属微粒子の製造方法 |
WO2007105656A1 (ja) * | 2006-03-09 | 2007-09-20 | N.E. Chemcat Corporation | 四面体パラジウム微粒子、および金属微粒子の製造方法 |
JP2012120981A (ja) * | 2010-12-08 | 2012-06-28 | Honda Motor Co Ltd | 酸化還元反応用合金触媒の製造方法 |
KR20160029790A (ko) * | 2013-07-01 | 2016-03-15 | 에꼴 뽈리떼끄닉 뻬데랄 드 로잔느 (으뻬에프엘) | 태양 전지 및 이를 제조하기 위한 공정 |
KR102258500B1 (ko) * | 2013-07-01 | 2021-06-01 | 에꼴 뽈리떼끄닉 뻬데랄 드 로잔느 (으뻬에프엘) | 태양 전지 및 이를 제조하기 위한 공정 |
Also Published As
Publication number | Publication date |
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EP1483050A1 (en) | 2004-12-08 |
EP1483050A4 (en) | 2009-12-09 |
US20030232721A1 (en) | 2003-12-18 |
WO2003064037A1 (en) | 2003-08-07 |
US6746597B2 (en) | 2004-06-08 |
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