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高比表面铀氧化物固体酸的制备及其催化乙醇脱水性能的研究 |
Preparation of Uranium Oxide-based Solid Acids with High Specific Surface Area and its Catalytic Performance for Ethanol Dehydration |
投稿时间:2024-04-08 修订日期:2024-05-07 |
DOI: |
中文关键词: 三氧化铀 酸改性 乙醇脱水 乙烯 |
英文关键词:uranium oxide acid modification ethanol dehydration ethylene |
基金项目:国家自然科学基金资助项目(22272074) |
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中文摘要: |
以未除去模板剂的高表面介孔氧化硅为主体,经模板交换同时引入UO22+及SO42-物种等过程,制得比表面高达215 m2·g-1的铀氧化物固体酸。XRD、SEM-EDS、FTIR及XPS分析结果表明,所得样品中的铀氧化物处于高分散状态,U为正六价;NH3-TPD研究结果显示,高分散态铀氧化物固体酸的总酸量高达6.02 mmol·g-1,为体相铀氧化物固体酸的23倍;反应温度为300℃、乙醇重时空速WHSV为2.5 h-1时,高分散态铀氧化物固体酸的乙醇转化率和乙烯选择性均为100%。在乙醇浓度为60 vol%,WHSV为2.5 h-1以及300℃反应条件下,高分散态铀氧化物表现出良好的酸催化稳定性:连续反应11 h,乙醇转化率保持在 100%,乙烯的选择性保持在 98.8%以上。 |
英文摘要: |
The uranium oxide solid acid with a surface ratio of up to 215 m2·g-1 was prepared by introducing UO22+ and SO42- species into high surface mesoporous silicon oxide with no template agent removed. XRD, SEM-EDS, FTIR and XPS analysis results show that the uranium oxides in the samples are highly dispersed and U is hexavalent. The results of NH3-TPD showed that the total acid content of highly dispersed uranium oxide solid acid was as high as 6.02 mmol·g-1, which was 23 times that of bulk phase uranium oxide solid acid. When the reaction temperature is 300℃ and the space velocity WHSV is 2.5 h-1, the ethanol conversion and ethylene selectivity of the highly dispersed uranium oxide solid acid are 100%. Under the conditions of ethanol concentration of 60 vol%, WHSV of 2.5 h-1 and 300℃, the highly dispersed uranium oxide showed good acid catalytic stability: the ethanol conversion remained at 100% and the ethylene selectivity remained above 98.8% after continuous reaction for 11 h. |
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