化工学报 ›› 2015, Vol. 66 ›› Issue (1): 105-113.DOI: 10.11949/j.issn.0438-1157.20140645

• 催化、动力学与反应器 • 上一篇    下一篇

棉杆活性炭负载Co-B催化剂催化硼氢化钠水解制氢的性能

曲健林1, 韩敏1, 张秀丽1, 徐秀峰2, 郭庆杰1   

  1. 1 青岛科技大学化工学院, 清洁化工过程山东省高校重点实验室, 山东 青岛 266042;
    2 烟台大学应用催化研究所, 山东 烟台 264005
  • 收稿日期:2014-04-23 修回日期:2014-10-21 出版日期:2015-01-05 发布日期:2015-01-05
  • 通讯作者: 郭庆杰
  • 基金资助:

    国家自然科学基金项目(21276129);青岛市应用基础研究计划项目(14-2-4-5-jch)。

Hydrogen generation by sodium borohydride hydrolysis on Co-B catalysts supported on cotton stalk-based activated carbon

QU Jianlin1, HAN Min1, ZHANG Xiuli1, XU Xiufeng2, GUO Qingjie1   

  1. 1 Key Laboratory of Clean Chemical Processing of Shandong Province, School of Chemical Engineering, Qingdao University of Science & Technology, Qingdao 266042, Shandong, China;
    2 Institute of Applied Catalysis, Yantai University, Yantai 264005, Shandong, China
  • Received:2014-04-23 Revised:2014-10-21 Online:2015-01-05 Published:2015-01-05
  • Supported by:

    supported by the National Natural Science Foundation of China (21276129) and the Qingdao Application Foundation Research Project (14-2-4-5-jch).

摘要:

采用棉杆生物质废弃物为原料、H3PO4为活化剂, 在流化床中化学活化制备棉杆活性炭, 并将其作为载体负载Co-B组分, 制备了棉杆活性炭基Co-B催化剂(Co-B/C)。以该催化剂应用于硼氢化钠水解制氢, 系统考察了活性炭活化条件(活化温度、活化时间、活化剂用量mH3PO4/mCS)、水解反应温度及催化剂循环使用次数对催化产氢性能的影响。同时, 使用N2物理吸附、FTIR、XRD和SEM等技术对活性炭载体及催化剂进行了表征。结果表明:在活化温度500℃、活化时间1 h、mH3PO4/mCS为0.75条件下制得的活性炭载体, 负载14.5%Co的催化剂表现出最佳催化性能:反应温度为25℃时, 平均产氢速率可以达到12.06 L·min-1·(g Co)-1, 催化剂表现了较高活性。催化产氢反应的活化能为44.61 kJ·mol-1。循环使用5次后, 催化剂仍保持初次活性的54%。

关键词: 活性炭, 催化剂载体, 活化条件, Co-B/C催化剂, 硼氢化钠, 制氢

Abstract:

Cotton stalk-based activated carbons were prepared by phosphoric acid activation of cotton stalks (CS) in a fluidized bed. The Co-B catalysts supported on cotton stalk-based activated carbon were generated by the impregnation-chemical reduction method. Meanwhile, the prepared activated carbons and catalysts were characterized by nitrogen physisorption, FTIR, XRD and SEM. The effects of activation reaction parameters, reaction temperature and recycle times on hydrogen generating performance of the activated carbons supported Co-B catalysts were investigated. The optimal activation temperature, activation time and amount of activator (mH3PO4/mCS) for activation of cotton stalk were 500℃, 1 h and 0.75, respectively. Under these conditions, the as-prepared Co-B/C catalyst with 14.5% (mass) Co exhibited the best hydrogen generating performance with an average rate of hydrogen generation up to 12.06 L·min-1·(g Co)-1 at 25℃. Activation energy of hydrogen generation reaction on such catalyst was estimated to be 44.61 kJ·mol-1. After five cycles, the catalyst retained 54% initial activity, exhibiting high activity and stability.

Key words: activated carbon, catalyst support, activation condition, Co-B/C catalyst, sodium borohydride, hydrogen production

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