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ID 109942
著者
杉山, 茂 Department of Advanced Materials, Institute of Technology and Science, The University of Tokushima|Department of Resource Circulation Engineering, Center for Frontier Research of Engineering, The University of Tokushima|Department of Chemical Science and Technology, The University of Tokushima 徳島大学 教育研究者総覧 KAKEN研究者をさがす
バンドウ, タクヤ Department of Chemical Science and Technology, The University of Tokushima
セノ, ユウスケ Department of Chemical Science and Technology, The University of Tokushima
ワタナベ, エミコ Department of Chemical Science and Technology, The University of Tokushima
中川, 敬三 Department of Advanced Materials, Institute of Technology and Science, The University of Tokushima|Department of Resource Circulation Engineering, Center for Frontier Research of Engineering, The University of Tokushima|Department of Chemical Science and Technology, The University of Tokushima KAKEN研究者をさがす
加藤, 雅裕 Department of Advanced Materials, Institute of Technology and Science, The University of Tokushima|Department of Chemical Science and Technology, The University of Tokushima 徳島大学 教育研究者総覧 KAKEN研究者をさがす
外輪, 健一郎 Department of Advanced Materials, Institute of Technology and Science, The University of Tokushima|Department of Resource Circulation Engineering, Center for Frontier Research of Engineering, The University of Tokushima|Department of Chemical Science and Technology, The University of Tokushima KAKEN研究者をさがす
カトウ, ユウキ Coporate Research Laboratories, Mitsubishi Rayon Co. Ltd.
アキハラ, シュウジ Coporate Research Laboratories, Mitsubishi Rayon Co. Ltd.
ニノミヤ, ワタル Coporate Research Laboratories, Mitsubishi Rayon Co. Ltd.
キーワード
Oxidative Esterification
Propionaldehyde
Methyl Propionate
Palladium Catalyst
Pressurized Oxygen
資料タイプ
学術雑誌論文
抄録
The optimization of the oxidative esterification of propionaldehyde to methyl propionate using a supported palladium catalyst in methanol under heavy-metal-free and pressurized-oxygen conditions, which we recently reported in a previous paper, were carried out together with a study of the reaction route, the nature of the catalytic active sites, and the effect of the support. In our previous paper, we reported significantly improved activity for oxidative esterification using commercially available 5%Pd/Al2O3 at 1.5 MPa of O2 gas and 333 K and emphasized that the doping of 5%Pd/Al2O3 with lead was not needed for the reaction system, but we could not improve the activity that was reported when using 5%Pd/γ-Al2O3 doped with 5% Pb (a 93.2% conversion of propionaldehyde, 76.8% selectivity for methyl propionate and a 71.6% yield of methyl propionate) at 0.3 MPa of O2 gas and 353 K, as reported by another laboratory. In the present study, however, we exceeded those values and obtained a 98.3% conversion of propionaldehyde, 75.3% selectivity for methyl propionate and a 74.0% yield of methyl propionate using 5%Pd/γ-Al2O3 undoped with Pb at 1.5 MPa of O2 gas and 333 K. It should be noted that, in the preparation of the present 5%Pd/γ-Al2O3, Pd was doped onto Al2O3 that had been previously treated with aqueous NaOH. Another active alumina support,η-Al2O3, prepared from boehmite, afforded activity that was substantially lower than that of γ-Al2O3 and depended on the calcination temperature of boehmite to η-Al2O3. When using various concentrations of CH3OH in the aqueous reaction solution, the oxidative esterification proceeded through the formation of propionic acid. To determine why the Al2O3 support afforded better activity than the active carbon support, Pd/Al2O3 and Pd/C catalysts were examined by XAFS (X-ray absorption fine structure). XAFS revealed that Pd on Al2O3 shows a better redox nature than Pd on C, which resulted in activity on Pd/Al2O3 that was better than that on Pd/C.
掲載誌名
Journal of Chemical Engineering of Japan
ISSN
00219592
cat書誌ID
AA00709658
46
7
開始ページ
455
終了ページ
460
並び順
455
発行日
2013
備考
Copyright © 2013 The Society of Chemical Engineers, Japan
EDB ID
出版社版DOI
出版社版URL
フルテキストファイル
言語
eng
著者版フラグ
著者版
部局
理工学系