成果報告書詳細
管理番号20110000001084
タイトル*平成22年度中間年報 新エネルギー技術研究開発 バイオマスエネルギー等高効率転換技術開発(先導技術開発) セルロース系バイオマスエタノールからプロピレンを製造するプロセス開発
公開日2011/7/28
報告書年度2010 - 2010
委託先名触媒技術研究組合 独立行政法人産業技術総合研究所 国立大学法人東京工業大学 国立大学法人広島大学
プロジェクト番号P07015
部署名新エネルギー部
和文要約和文要約等以下本編抜粋:1. 研究開発の内容及び成果等 本研究では、2015~2020年頃の実用化をめざし、セルロース系エタノールからプロピレンを製造するための触媒開発、反応および分離精製プロセス開発を行う。本事業の目的を達成するための主な開発項目は、1)エタノールを直接プロピレンへ化学変換する高性能で長寿命の触媒を開発し、その評価を行うこと、2)原料中に存在する触媒被毒成分の分離除去、およびポリマーグレードのプロピレンを触媒反応生成物から分離精製する技術を開発すること、3)上記触媒および分離精製工程を含むコスト競争力のあるプロセスを開発し、ベンチプラントの設計を行うことである。
英文要約Title: Development of technologies to produce propylene from cellulosic ethanol (FY2008-2011) FY2010 Annual Report.
(1) Catalyst stability of MFI-type H-ZSM-5 zeolite was found to be improved by modification by zirconium oxide. Addition of alkali-earth metals such as Mg to La-modified zeolites caused further neutralization of strong acid sites of the zeolites, leading to predominant formation of ethylene over propylene. Moderate additive effects were observed by modification of zeolites by rare-earth phosphates and ethylene selectivity increased, while propylene selectivity decreased gradually, as the reaction proceeded. Similar effects were obtained by transition-metal phosphates-modified zeolites, however, after water treatment, surface acidity changed and both ethylene and propylene selectivities gently increased. (2) SAPO-34 has the advantage of high selectivity for propylene. We have found that inactivation of external active sites of SAPO-34 with small particle sizes can improve the propylene yield in the conversion of ethanol. The most active catalyst exhibited the highest propylene yield of 54% at 400℃under these conditions, the ethylene yield was 24%. (3) Extensive studies were carried out for development of non-silica catalyst with high propylene yield in the conversion of ethanol to propylene. The activity and stability of non-silica catalyst were improved by optimization of the catalyst composition and the preparation method. The improved catalyst with high surface area showed over 50% of the propylene yield and about 15 hours of the catalytic stability. The selectivity to propylene was improved by the addition of water and the increase in reaction pressure to 0.2-0.5 MPaG. A recycle system of an intermediate compound yielding propylene was also developed on the basis of the reaction mechanism. Dimethylsulfide and dimethylsulfoxide possibly included in bio-ethanol little affected the catalytic activity of non-silica catalyst. (4) Adsorptive desulfurization of propylene derived from bioethanol was examined. Among the tested adsorbents, porous iron oxide and porous alumina-zeolite complex modified with alkali metal were found to be most effective for the selective removal of hydrogen sulfide from propylene. (5) Selective membrane separation of saturated water vapor from propylene has been examined using a carbon hollow fiber membrane. It was confirmed that the carbon membrane showed superior olefin gas dehydration performance. (6) A bench scale reactor (capacity of 100kg/d bio-ethanol) has been designed to produce propylene with its yield of 35% or more from ethanol by using non-silica catalysts. Designed dimensions of packed bed reactors are as follows: (case-1) reactor diameter=12.5 cm, bed height=120cm, (case-2) reactor diameter=25cm, bed height=30cm. (7) Reaction product from micro-size reactor contains propylene, ethylene, propane, etc. Also propylene distillation unit completed to separate propylene from reaction product and obtain 99.5wt propylene.
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