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題 名 | Influence of Secondary Metal Oxide Additives on Molecular Structure and Reactivity of V[feaf]O邚/SnO[feaf]/SiO[feaf] Catalysts during Methanol Oxidation=金屬氧化物添加物對V[feaf]O邚/SnO[feaf]/SiO[feaf]觸媒於甲醇氧化反應中之分子結構與反應活性之影響 |
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作 者 | 鄭紀民; 陳松青; 劉玉城; | 書刊名 | Journal of the Chinese Institute of Chemical Engineers |
卷 期 | 30:4 1999.07[民88.07] |
頁 次 | 頁319-327 |
分類號 | 460.02 |
關鍵詞 | 金屬氧化物添加物; 觸媒; 甲醇氧化反應; 分子結構; 反應活性; Supported vanadium oxide; Mixed oxide support; In situ raman; Reducibility; Surface acidity; Methanol oxidation; |
語 文 | 英文(English) |
中文摘要 | 由添加CrO3,Nb2O5,WO3添加物於被擔持釩氧化物覆載於混合氧化物載體觸媒中之拉 曼光譜得知CrO3形成一表面CrO3層於觸媒表面,而Nb2O5及WO3分別形成Nb2O5及WO3顆粒於觸 媒表面。表面CrO3分子與被擔持釩氧化物覆載於混合氧化物載體觸媒之V-O-Sn橋式鍵結之 相互作用使得表面釩氧化物在甲醇氧化反應條件下完全還原。由於無V+5原子狀態於反應過程 中導致甲醇氧化反應之活性降低。形成Nb2O5及WO3顆粒於觸媒表面亦降低甲醇氧化反應之活 性。添加不同添加物會對觸媒之表面酸性基位有不同之影響,但形成新表面酸性基位對甲醇氧 化反應之反應機制並無明顯之變化及影響,通常甲醇氧化反應只需單一氧化/還原基位即可進 行反應。由溫控程式還原實驗可知,添加物本身之還原能力對被擔持釩氧化物於此混合氧化物 載體觸媒之還原能力有影響作用。 |
英文摘要 | In situ Raman studies of the CrO3, Nb2O5, and WO3-V2O5/SnO2/SiO2 catalysts have revealed that chromium oxide forms a surface CrO3 overlayer and niobium oxide and tungsten oxide form bulk Nb2O5 and WO3 particles, respectively, on the surface. The interaction of the surface CrO3 species with the V-O-Sn bridging bond in the V2O5/SnO2/SiO2 catalyst induces the total reduction of the surface vanadium oxide species during methanol oxidation. The absence of V+5 atom in the catalyst during reaction conditions results in a lower reactivity of the methanol oxidation reaction. The formation of bulk Nb2O5 and WO3 particles on the V2O5/ SnO2/SiO2 surface also decrease methanol oxidation reactivity. The formation of new surface acid sites on the promoted-V2O5/SnO2/SiO2 catalysts does not alter the reaction mechanisms toward the acid site's product (CH3OCH3), and only one site (redox) is needed to perform the methanol oxidation reaction. TPR studies indicate that the reducibility of the surface vanadium oxide species is affected by the reducibility of the secondary metal oxide. |
本系統中英文摘要資訊取自各篇刊載內容。