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化学工业与工程 2013, Vol. 30 Issue (4) :16-22    DOI:
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甘油氢解合成1,2-丙二醇铜锌铝催化剂的性能
 李莉, 杨娟, 于磊, 陈吉祥
天津大学化工学院,天津 300072
Performance of Cu-Zn-Al Catalyst for Hydrogenolysis of Glycerol to 1,2-Propanediol
 LI  Li, YANG  Juan, YU  Lei, CHEN  Ji-Xiang
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

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摘要 采用共沉淀法制备了铜锌铝类水滑石前驱体,经焙烧和还原后制得铜基催化剂。采用XRD、H2-TPR、H2-TPD、NH3-TPD和CO2-TPD等表征手段并结合甘油氢解反应评价,研究了类水滑石前驱体的老化对催化剂结构和性能的影响,考察了反应条件对催化剂甘油氢解反应性能的影响。结果表明,老化有利于形成结构更为完整的类水滑石前驱体,但对铜物种的还原性能未造成显著影响。与由未老化前驱体制备的催化剂相比,由老化前驱体制备的铜锌铝催化剂具有较大Cu表面及较大酸量,但表面碱中心数量较低,从而该催化剂具有较好的甘油氢解活性及稳定性。在220 ℃、H2压力3.0 MPa、n(H2)/n(甘油)为18.9、甘油重时空速1.26 h-1及质量分数为60%甘油水溶液的条件下,经老化前驱体制备的铜锌铝催化剂上甘油转化率接近100%、1, 2-丙二醇选择性约为96%。
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李莉
杨娟
于磊
陈吉祥
关键词铜锌铝催化剂   类水滑石   甘油氢解   1, 2-丙二醇     
Abstract: Cu-Zn-Al and Cu-Zn-Al-no hydrotalcite precursors, which were respectively aged and un-aged during the preparation process, were prepared by coprecipitation. After the hydrotalcite precursors were calcined and reduced, Cu-based catalysts were obtained. The effect of ageing on the structure and performance of the catalysts for the hydrogenolysis of glycerol was studied by means of H2-TPR, XRD, H2-TPD, NH3-TPD and CO2-TPD and activity test. Also, the effect of the reaction conditions on the performance of Cu-Zn-Al catalyst was investigated. After calcination at 450 ℃, the hydrotalcite-like precursors were transformed to the mixed oxides without hydrotalcitelike structure, in which Cu species dispersed well. Cu-Zn-Al-no and Cu-Zn-Al had similar reducibility. After reduction at 270 ℃, the mixed oxides were converted to Cu-based catalysts. Compared with the Cu-Zn-Al-no, Cu-Zn-Al had larger active surface, more acid sites and less basic sites. Thus, in the hydrogenolysis of glycerol, the Cu-Zn-Al catalyst showed better activity, selectivity and stability than the Cu-Zn-Al-no catalyst. Under the condition of 220 ℃, 3.0 MPa H2 pressure, H2/glycerol molar ratio of 18.9, space velocity of 1.89 h-1 and 60%(mass fraction) glycerol aqueous solution, the Cu-Zn-Al catalyst gave glycerol conversion of 100% and 1,2-propanediol selectivity of 96%.
KeywordsCu-Zn-Al catalyst   hydrotalcite   glycerol hydrogenolysis   1,2-propanediol     
Received 2012-06-05;
Corresponding Authors: 陈吉祥,电话:(022) 27890865, E-mail: jxchen@tju.edu.cn。     Email: jxchen@tju.edu.cn
About author: 李莉(1986-),女,硕士研究生,现从事多相催化剂研究。
引用本文:   
李莉, 杨娟, 于磊, 陈吉祥.甘油氢解合成1,2-丙二醇铜锌铝催化剂的性能[J].  化学工业与工程, 2013,30(4): 16-22
LI Li, YANG Juan, YU Lei, CHEN Ji-Xiang.Performance of Cu-Zn-Al Catalyst for Hydrogenolysis of Glycerol to 1,2-Propanediol[J].  Chemcial Industry and Engineering, 2013,30(4): 16-22
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