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CuO基金属氧化物液相催化转化纤维素制备燃料和化学品的研究
Alternative TitleCatalytic conversion of cellulose to fuels and chemicals over CuO-based metal oxide catalysts in liquid phase
吴艳华
Subtype硕士
Thesis Advisor苏发兵
2013-05-01
Degree Grantor中国科学院研究生院
Degree Discipline材料学
Keyword纤维素   催化转化   甲醇   cuo基催化剂
Abstract本论文采用甲醇重整耦合纤维素转化的方法,以CuO基金属氧化物为催化剂,实现了纤维物的高效催化转化。在这一转化过程中,甲醇重整产生的氢气可以直接用于纤维素的进一步加氢。CuO基金属氧化物既催化了甲醇重整反应产生氢气,也催化了纤维素转化反应。本研究为纤维素催化转化制备燃料和化学品提供了高效经济的新路径。 论文的主要研究内容及创新性成果如下: 1.以甲醇为反应介质,以不同质量比的CuO/Al2O3二元金属氧化物为催化剂,进行了纤维素转化活性评价。结果显示,气体产物中主要组分H2的含量可以达到50 %以上。催化剂中CuO/Al2O3的质量比对于液相产物的分布有一定的影响,其中,当催化剂中CuO质量分数高于75 %时,主要的液相产物为醇类,当CuO百分含量低于75 %时,主要的液相产物为醚类和烷烃。 2.以甲醇为反应介质,以CuO-MO/Al2O3(M=Ce,Mg,Mn,Ni,Zn)三元金属氧化物为催化剂,进行了纤维素转化活性评价。结果显示,气体产物中主要组分H2的含量可以达到60 %以上,液相产物中的主要组分为C4-C7醇。第三组分的添加对于液相产物的分布有一定的影响,其中,CeO,MgO和ZnO的添加提高了液相产物中C4-C7醇的收率,而NiO的添加促进了甲酯类和呋喃类等不饱和含氧有机物的生成。CuO-ZnO/Al2O3催化剂展示了最好的催化活性,气体产物和液相产物的收率均为最高,液相产物中C4-C7醇的相对含量能够达到95.3 %; 3.以甲醇为反应介质,考察了反应温度、反应时间以及纤维素加入量对CuO-ZnO/Al2O3催化转化纤维素的活性影响。优化的反应条件为:反应温度为280 °C,反应时间为120 min,纤维素加入量为0.5 g。在4次循环反应实验中,纤维素催化转化的气体产物和液体产物的分布均变化不大,液相产物中C4-C7醇的收率及相对含量也都保持稳定,这说明CuO-ZnO/Al2O3催化剂具有很好的稳定性和循环使用性能。
Other AbstractThis work demonstrates the efficient catalytic conversion of cellulose by coupling the reaction of cellulose conversion with the reforming reaction of methanol over CuO-based catalysts. In this process, the in-situ regenerated H2 in the methanol reforming reaction can be used in the hydrogenation reaction of cellulose directly. The CuO-based catalysts catalyze both the methanol reforming reaction and cellulose conversion reaction. This work provides a cost-effective route to convert abundant renewable cellulose to liquid fuels. The major work and innovative results for this dissertation are as follows: 1. Catalytic conversion of cellulose was evaluated over CuO/Al2O3 binary metal oxide catalysts with different mass ratios in the presence of methanol. The results show that the content of H2 in the gas products is above 50%. The mass ratio of the CuO/Al2O3 catalyst have a certain influence on the distribution of the liquid product, and wherein, when the CuO mass content is above 75 %, the main liquid product is alcohols; when the CuO mass content is less than 75 %, the main liquid product is ethers and alkanes. 2. Catalytic conversion of cellulose was evaluated over CuO-MO/Al2O3 (M=Ce, Mg, Mn, Ni, Zn) metal oxide catalysts in the presence of methanol. The results show that the content of H2 in the gas product is above 60%, and the C4-C7 alcohols are the main liquid products. The addition of the third metal component has a certain impact on the distribution of the liquid products, wherein, the addition of CeO, MgO and ZnO can improve the yield of C4-C7 alcohols in the liquid products, while the addition of NiO promote the formation of unsaturated oxygenated organic component such as methyl esters and furans. CuO-ZnO/Al2O3 catalyst shows the best catalytic activity, in which the yield of gas and liquid products are the highest, and the relative content of C4-C7 alcohol in the liquid product can be as high as 95.3 %. 3. The effects of reaction temperature, reaction time, and cellulose amount on catalytic conversion of cellulose over CuO-ZnO/Al2O3 catalyst in the presence of methanol were studied. The optimized reaction conditions are as follows: the reaction temperature= 280 °C, the reaction time= 120 min, and the cellulose mount= 0.5 g. Four cycles reaction results show that the the distribution of gas and liquid products has no obvious change, and the yield and relative content of the C4-C7 alcohol in the liquid product are also stable, indicating CuO-ZnO/Al2O3 catalyst is stabe and reusable in the reaction conditions.
Pages60
Language中文
Document Type学位论文
Identifierhttp://ir.ipe.ac.cn/handle/122111/8300
Collection研究所(批量导入)
Recommended Citation
GB/T 7714
吴艳华. CuO基金属氧化物液相催化转化纤维素制备燃料和化学品的研究[D]. 中国科学院研究生院,2013.
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