Carrier effect on the nature of V4+ and active oxygen species in vapor-phase oxidation of butadiene over supported divanadium pentaoxide catalysts.
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概要
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The reactivity of V<SUP>4+</SUP> with gaseous oxygen formed on various kinds of supported V<SUB>2</SUB>O<SUB>5</SUB> catalysts has been investigated by ESR. The results are discussed as carrier effect in relation to the selectivity for maleic anhydride formation during the course of the vapor-phase oxidation of butadiene. V<SUP>4+</SUP> formed on Al<SUB>2</SUB>O<SUB>3</SUB> (V/Al≤10/90 atom ratio) and MgO (V/Mg≤30/70) showed a hyperfine ESR structure and was hardly oxidized whereas V<SUP>4+</SUP> formed on SiO<SUB>2</SUB> (V/Si≥5/95) had the singlet ESR signal and was easily oxidized. Formation of these two kinds of V<SUP>4+</SUP> was observed on V<SUB>2</SUB>O<SUB>5</SUB>–Al<SUB>2</SUB>O<SUB>3</SUB> (V/Al≥20/80). They were similarly observed in the case of V<SUB>2</SUB>O<SUB>5</SUB>-TiO<SUB>2</SUB>, but some portion of V<SUP>4+</SUP> having the hyperfine structure was also oxidized. The selectivity was high over the catalysts forming the reactive V<SUP>4+</SUP> as compared with those forming the unreactive one. The reactive V<SUP>4+</SUP> was shown by X-ray diffraction to be preferentially formed in crystalline V<SUB>2</SUB>O<SUB>5</SUB>. Study of the reduction and reoxidation of unsupported crystalline V<SUB>2</SUB>O<SUB>5</SUB> by means of IR and the effect of addition of alkali metal oxide on the catalytic activity of the supported V<SUB>2</SUB>O<SUB>5</SUB> were discussed. The important role of double bond type lattice oxygen V=O in maleic anhydride formation was proposed.
- 公益社団法人 日本化学会の論文
著者
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Akimoto Masamichi
Department Of Applied Chemistry And Biotechnology Faculty Of Engineering Niigata Institute Of Techno
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Echigoya Etsuro
Department of Chemical Engineering, Tokyo Institute of Technology
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Usami Masahiro
Department of Chemical Engineering, Tokyo Institute of Technology
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