Co/La-Ga-O复合氧化物用于催化二氧化碳加氢制乙醇
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  • 英文篇名:Direct synthesis of ethanol via CO_2 hydrogenation over the Co/La-Ga-O composite oxide catalyst
  • 作者:郑晋楠 ; 安康 ; 王嘉明 ; 李晶 ; 刘源
  • 英文作者:ZHENG Jin-nan;AN Kang;WANG Jia-ming;LI Jing;LIU Yuan;School of Chemical Engineering,Tianjin University Tianjin Key Laboratory of Applied Catalysis Science and Technology;Collaborative Innovation Center of Chemical Science and Engineering ( Tianjin);
  • 关键词:二氧化碳加氢 ; 乙醇合成 ; 钙钛矿型氧化物 ; ;
  • 英文关键词:carbon dioxide hydrogenation;;ethanol synthesis;;perovskite-type oxide;;cobalt;;gallium
  • 中文刊名:RLHX
  • 英文刊名:Journal of Fuel Chemistry and Technology
  • 机构:天津大学化学工程学院天津市应用催化科学与工程重点实验室;天津化学化工协同创新中心;
  • 出版日期:2019-06-25 14:08
  • 出版单位:燃料化学学报
  • 年:2019
  • 期:v.47
  • 基金:国家自然科学基金(21872101,21576192)资助~~
  • 语种:中文;
  • 页:RLHX201906007
  • 页数:12
  • CN:06
  • ISSN:14-1140/TQ
  • 分类号:67-78
摘要
以LaCo_(1-x)Ga_xO_3为前驱体,还原后得到的Co/La_2O_3-La_4Ga_2O_9复合氧化物催化剂,用于CO_2加氢直接制乙醇。通过XRD、XPS、TPD和TEM等技术对催化剂结构进行了表征,采用微型固定床反应器在230-290℃、3 MPa、空速(GHSV)为3000 mL/(g_(cat)·h)和H_2/CO_2进料物质的量比为3.0的条件下,考察了该Co/La-Ga-O复合氧化物用于CO_2加氢制乙醇的催化性能。结果显示,该Co/La-Ga-O复合氧化物催化剂对生成乙醇具有很高的选择性。与LaCoO_3相比,Ga的掺杂可抑制甲烷的形成,促进醇类(特别是乙醇)的生成。当Co/Ga比为7∶3时,还原后的LaCo_(1-x)Ga_xO_3催化剂体现出最好的催化性能,CO_2转化率为9.8%,总醇选择性达到74.7%,其中,液相产物中的乙醇质量分数可达到88.1%。基于实验结果推测,该催化剂上Co~0和Co~(δ+)的协同作用促使CO_2选择性加氢生成乙醇。
        A new Co/La_2 O_3-La_4 Ga_2 O_9 catalyst was prepared by reducing LaCo_(1-x)Ga_xO_3 perovskite and used in the direct synthesis of ethanol from CO_2 hydrogenation. The composite catalyst was characterized by XRD,XPS,TPD and TEM and its catalytic performance in CO_2 hydrogenation was investigated in a micro fixed-bed reactor operated at 230-290 ℃,3 MPa,gas hourly space velocity( GHSV) of 3000 mL/( gcat·h) and H_2/CO_2 molar ratio of 3.0. The results indicate that the Co/La-Ga-O composite oxide catalyst exhibits high selectivity to ethanol in CO_2 hydrogenation. In comparison with the LaCoO_3 catalyst,the incorporation of Ga dopant can inhibit the formation of CH4 and then promote the production of alcohols,especially ethanol. With a Co/Ga atomic ratio of7 ∶3,the Co/La-Ga-O composite oxide catalyst displays the best performance in CO_2 hydrogenation,with a CO_2 conversion of 9.8%,a selectivity of 74.7% to total alcohols and ethanol content of 88.1%( mass ratio) in the alcohols mixture. On the basis of the experimental results,it is speculated that the synergistic effect of surface Co~0 and Co~(δ+) may contribute to the excellent performance of the Co/La_2 O_3-La_4 Ga_2 O_9 catalyst in CO_2 hydrogenation to ethanol.
引文
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