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以类水滑石为前体的铜基催化剂催化甘油氢解反应 被引量:1

Hydrogenolysis of Glycerol to 1,2-Propanediol on Cu-Based Catalysts Derived from Hydrotalcite-Like Precursors
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摘要 以Cu-Zn-Al和Cu-Mg-Al类水滑石为前体经焙烧、还原制备了铜基催化剂,采用XRD、H2-TPR、N2吸附、H2-TPD、NH3-TPD、CO2-TPD及活性评价等方法,研究了M2+离子(M2+=Zn2+或Mg2+)及n(M2+)/n(Al3+)比对催化剂结构和甘油氢解反应性能的影响。结果表明,经450℃焙烧后,类水滑石转变为由尖晶石和/或氧化物组成的氧化态前驱体,再经270℃还原后制得高分散Cu催化剂。随氧化铝含量提高,催化剂比表面及酸量增加。Cu-Zn-Al催化剂表面氢吸附量大于CuMg-Al。Cu-Mg-Al催化剂碱性强于Cu-Zn-Al。Cu-Zn-Al[n(Cu)∶n(Zn)∶n(Al)=1∶1∶4]催化剂具有较佳甘油氢解活性及1,2-丙二醇选择性,这与其具有较多表面铜中心、较大酸量及Zn物种参与氢吸附有关。此外,Cu-Mg-Al催化剂表面铜中心和碱中心可能存在协同作用促进甘油氢解反应。 Cu-Zn-Al and Cu-Mg-Al catalysts were prepared from hydrotalcite-like precursors after calcination and reduction. The effect of M2 +( M = Zn or Mg) and M2 +/ Al3 +ratio on the catalyst structure and performance were investigated by means of XRD,H2-TPR,N2-sorption,H2-TPD,NH3-TPD,CO2-TPD and activity test. The hydrotalcite-like precursors were transformed to the spinel and / or metal oxides after calcination at 450 ℃,from which the highly dispersed Cu-based catalysts were prepared after reduction at 270 ℃. Compared with the Cu-Mg-Al catalysts,the Cu-Zn-Al catalysts had more amounts of adsorbed hydrogen due to the role of Zn species. With increasing Al2O3 content,the specific surface area and acid amount increased. The Cu-Mg-Al catalysts had more basic sites than the Cu-Zn-Al catalysts. In the hydrogenolysis of glycerol,Cu-Zn-Al[n( Cu) ∶ n( Zn) ∶ n( Al) = 1∶ 1∶ 4] had the highest activity and selectivity to 1,2-propanediol,which is due to the largest amounts of surface Cu and acid sites. For the CuMg-Al catalysts,there may be a synergism between the Cu and basic sites.
作者 田沙沙 杨娟 陈吉祥 Tian Shasha, Yang Juan, Chen Jixiang (School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China)
出处 《化学工业与工程》 CAS CSCD 2015年第2期25-30,共6页 Chemical Industry and Engineering
关键词 类水滑石 甘油氢解 1 2-丙二醇 铜镁铝 铜锌铝 hydrotalcite-like compound glycerol hydrogenolysis 1 2-propanediol Cu-Mg-Al catalyst Cu-Zn-Al catalyst
作者简介 田沙沙(1988一),女,硕士生,从事多相催化加氢研究。 通信作者:陈吉祥,电话:(022)27890865,E-mail:jxchen@tju.edu.cn。
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