制备方法对Ni/ZnO催化丙三醇重整-氢解性能的影响

采用浸渍法、共沉淀法、水热法和碳微球硬模板法制备了Ni/ZnO催化剂,运用X射线衍射、程序升温还原、透射电子显微镜和氢滴定等手段对其进行了表征,并用于连续固定床反应器中无外加氢气条件下的丙三醇重整-氢解反应.结果表明,在较低空速下,生成的1,2-丙二醇（1,2-PDO）易在Ni分散度较高的催化剂上进一步裂解为乙醇和气相产物;而在较高空速下,其选择性受制于中间产物丙酮醇的加氢.在优化的空速下,Ni分散度越高越有利于1,2-PDO的生成.在Ni分散度最高的Ni/ZnO催化剂上,当丙三醇质量空速为0.84h-1时,1,2-PDO选择性最高,为54.9%,丙三醇转化率为85.4%....

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Bibliographic Details
Published in催化学报 Vol. 33; no. 8; pp. 1266 - 1275
Main Author 胡基业 刘晓钰 王彬 裴燕 乔明华 范康年
Format Journal Article
LanguageChinese
Published 复旦大学化学系上海市分子催化和功能材料重点实验室,上海,200433 2012
Subjects
1,2-丙二醇
丙三醇
分散度
氢解
氧化锌
重整
镍
1,2-丙二醇
重整
丙三醇
分散度
氢解
镍
氧化锌
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ISSN0253-9837
1872-2067
DOI10.1016/S1872-2067(11)60405-1

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Summary:采用浸渍法、共沉淀法、水热法和碳微球硬模板法制备了Ni/ZnO催化剂,运用X射线衍射、程序升温还原、透射电子显微镜和氢滴定等手段对其进行了表征,并用于连续固定床反应器中无外加氢气条件下的丙三醇重整-氢解反应.结果表明,在较低空速下,生成的1,2-丙二醇（1,2-PDO）易在Ni分散度较高的催化剂上进一步裂解为乙醇和气相产物;而在较高空速下,其选择性受制于中间产物丙酮醇的加氢.在优化的空速下,Ni分散度越高越有利于1,2-PDO的生成.在Ni分散度最高的Ni/ZnO催化剂上,当丙三醇质量空速为0.84h-1时,1,2-PDO选择性最高,为54.9%,丙三醇转化率为85.4%.
Bibliography:HU Jiye, LIU Xiaoyu, WANG Bin, PEI Yan, QIAO Minghua＊, FAN Kangnian Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University Shanghai 200433, China
The catalytic conversion of glycerol to 1,2-propanediol （1,2-PDO） is generally conducted batch-wise in an autoclave in the pres- ence of high pressure H2. The reforming and hydrogenolysis of glycerol to 1,2-PDO over Ni/ZnO catalysts in a continuous flow fixed-bed reactor without added H2 was reported. The Ni/ZnO catalysts were prepared by wetness impregnation （WI）, co-precipitation （CP）, hydro- thermal treatment （HT）, and carbon microsphere hard-templating （CT） methods. The catalysts were characterized by X-ray diffraction （XRD）, temperature-programmed reduction （TPR）, transmission electron microscopy （TEM）, and H2 titration. At a low weight hourly space velocity （WHSV） of glycerol, the 1,2-PDO produced got degraded to ethanol and gas phase products over catalysts with high Ni dispersion, while at a high
ISSN:0253-9837
1872-2067
DOI:10.1016/S1872-2067(11)60405-1