CeMn/γ-Al2O3催化剂制备及催化降解乙酸乙酯性能
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常州大学石油化工学院

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Preparation of CeMn/γ-Al2O3 catalyst and catalytic degradation performance of ethyl acetate
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School of Petrochemical Engineering,Changzhou University,Changzhou

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    摘要:

    以硝酸铈、硝酸锰为原料,NaOH为沉淀剂,采用共沉淀法制备Ce1Mn3前驱体,通过与纳米氧化铝胶干粉混捏煅烧制备复合金属氧化物催化剂Ce1Mn3-x/γ-Al2O3〔x为Ce1Mn3前驱体粉末质量(g),取值为1、3、5、7、9,原料总质量10 g〕,采用XRD、BET和SEM对催化剂进行表征,通过固定床反应器考察其对气态低浓度乙酸乙酯(体积分数1000 ppm)的催化降解性能,并探究水蒸气对反应的影响和48 h催化稳定性。结果表明,γ-Al2O3的混捏并不改变Ce1Mn3物相。相较于Ce1Mn3,Ce1Mn3-x/γ-Al2O3的比表面增大(由38.55 m2/g增加至60.03~204.79 m2/g),介孔数量明显增加。Ce1Mn3氧化物结合在γ-Al2O3表面,暴露出的Ce1Mn3氧化物颗粒样貌更加细小且分散。Ce1Mn3与氧化铝溶胶干粉混捏质量比为7∶3时,制备的Ce1Mn3-7/γ-Al2O3催化活性最高,在空速(GHSV)15000 mL/(g·h)条件下,乙酸乙酯降解率90%的温度(T90)为164 ℃。载体γ-Al2O3和加入水蒸气均有利于乙酸乙酯在低温下(<120 ℃)的降解,促进降解中间体乙酸和乙醇生成,导致最终T90降低。在180 ℃、48 h不含水蒸气的反应气氛测试中,Ce1Mn3-7/γ-Al2O3催化剂能始终保持99%以上的乙酸乙酯降解率。

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    Ce1Mn3 precursor was prepared by co precipitation method using cerium nitrate and manganese nitrate as raw materials, NaOH as precipitant. The composite metal oxide catalyst Ce1Mn3-x/γ-Al2O3 was prepared by mixing and calcining with nano alumina gel powder. X is the mass of Ce1Mn3 precursor powder (g), with values of 1, 3, 5, 7, and 9, and a total raw material mass of 10 g. The catalyst was characterized by XRD, BET and SEM, and its catalytic degradation performance on gaseous low concentration ethyl acetate (volume fraction 1000 ppm) was investigated by a fixed bed reactor. The effect of water vapor on the reaction and 48 hour catalytic stability were also explored. Compared with Ce1Mn3, the specific surface area of Ce1Mn3-x/γ-Al2O3 increases from 38.55 m2/g to 60.03~20.79 m2/g, and the number of mesopores significantly increases. Ce1Mn3 oxide is bound to the surface of γ-Al2O3, and the exposed Ce1Mn3 oxide particles have a finer and more dispersed morphology. When the mass ratio of Ce1Mn3 to alumina sol dry powder is 7:3, Ce1Mn3-7/γ-Al2O3 has the highest catalytic activity. Under the condition of space velocity (GHSV) of 15000 mL/(g·h), the degradation rate of ethyl acetate reaches 90% at 164 ℃ (T90). Both the carrier γ-Al2O3 and the addition of water vapor are beneficial for the degradation of ethyl acetate at low temperatures (<120 ℃), promoting the generation of degradation intermediates acetic acid and ethanol, resulting in a decrease in the final T90. In a reaction atmosphere test at 180 ℃ for 48 hours without water vapor, the Ce1Mn3-7/γ-Al2O3 catalyst can consistently maintain a degradation rate of over 99% for ethyl acetate.

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孙哲恺,张智宏,杜晓刚. CeMn/γ-Al2O3催化剂制备及催化降解乙酸乙酯性能[J].精细化工,2025,42(6):

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  • 收稿日期:2024-06-11
  • 最后修改日期:2024-08-06
  • 录用日期:2024-07-18
  • 在线发布日期: 2025-06-06
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