Selective reduction of nitrogen monoxide with hydrogen on Pt/Al2O3 containing a metal oxide.
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概要
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By using a three-way catalyst containing a metal oxide, NO can be selectively converted to N<SUB>2</SUB> and N<SUB>2</SUB>O without the formation of NH<SUB>3</SUB> even at the "rich" side of the air/fuel ratio. In order to elucidate the mechanism of this action of the added metal oxide, the NO–H<SUB>2</SUB> reaction on Pt–V<SUB>2</SUB>O<SUB>5</SUB>/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst was investigated using the pulse reaction technique. In the NO–H<SUB>2</SUB> reaction on Pt/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst, a significant amount of NH<SUB>3</SUB> was formed in the "rich" region of the reactants (H<SUB>2</SUB>/NO>1), although NO was completely removed. In the NO–H<SUB>2</SUB> reaction on the Pt–V<SUB>2</SUB>O<SUB>5</SUB>/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst, on the other hand, no NH<SUB>3</SUB> was formed even in the "rich" region of the reactants; in addition, NO was completely removed. During the NO–H<SUB>2</SUB> reaction on the Pt–V<SUB>2</SUB>O<SUB>5</SUB>/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst, the V<SUB>2</SUB>O<SUB>5</SUB> in the catalyst was found to be reduced from V<SUP>5+</SUP> to V<SUP>4+</SUP>. The reaction of NO with NH<SUB>3</SUB> and the reaction of NH<SUB>3</SUB> or H<SUB>2</SUB> with Pt–V<SUB>2</SUB>O<SUB>5</SUB> mixed catalysts for various states of mixing were also investigated. From these results, the NO–H<SUB>2</SUB> reaction on the Pt–V<SUB>2</SUB>O<SUB>5</SUB>/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst has been shown to be composed of the following three main steps: Step I, the formation of NH<SUB>3</SUB> by the reduction of NO with H<SUB>2</SUB> on Pt; Step II, the NO–NH<SUB>3</SUB> reaction on Pt to form N<SUB>2</SUB> or N<SUB>2</SUB>O; and Step III, the reduction of V<SUB>2</SUB>O<SUB>5</SUB> in the catalyst by H<SUB>2</SUB> which is accelerated by the "hydrogen spil-lover." In the NO–H<SUB>2</SUB> reaction on Pt/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst, NO is first reduced to NH<SUB>3</SUB> in Step I and the NO–NH<SUB>3</SUB> reaction in Step II follows. In the "rich" region, the formation of NH<SUB>3</SUB> takes place more readily than the subsequent NO–NH<SUB>3</SUB> reaction. In the NO–H<SUB>2</SUB> reaction on the Pt–V<SUB>2</SUB>O<SUB>5</SUB>/Al<SUB>2</SUB>O<SUB>3</SUB> catalyst, the formation of excess NH<SUB>3</SUB> is suppressed by the removal of hydrogen from Pt in Step III, and the NH<SUB>3</SUB> thus produced reacts with NO to form N<SUB>2</SUB> or N<SUB>2</SUB>O selectively in Step II. The rates of Steps I, II, and III were also discussed in terms of the structure of the catalysts and composition of the reactants.
- 公益社団法人 日本化学会の論文
著者
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MURAKAMI Yuichi
Department of Applied Chemistry, School of Engineering, Nagoya University
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Miyamoto Akira
Department Of Applied Chemistry Graduate School Of Engineering Tohoku University
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Murakami Yuichi
Department of Synthetic Chemistry, Faculty of Engineering, Nagoya University
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Kosaki Yukio
Department of Synthetic Chemistry, Faculty of Engineering, Nagoya University
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