催化学报 ›› 2007, Vol. 28 ›› Issue (7): 611-616.

• 研究论文 • 上一篇    下一篇

过渡金属阳离子预处理对活性炭催化性能的提高

Sahar A. EL-MOLLA1, Gamil A. EL-SHOBAKY2, Sohair A. SAYED AHMED2   

  1. 1 艾因沙姆萨大学教育学院化学系, 开罗 11566, 埃及; 2 国家研究中心, 开罗 12622, 埃及
  • 收稿日期:2007-07-25 出版日期:2007-07-25 发布日期:2011-07-25

Catalytic Promotion of Activated Carbon by Treatment with Some Transition Metal Cations

Sahar A. EL-MOLLA1, Gamil A. EL-SHOBAKY2, Sohair A. SAYED AHMED2   

  1. 1 Chemistry Department, Faculty of Education, Ain Shams University, Cairo 11566, Egypt; 2 National Research Center, Cairo 12622, Egypt
  • Received:2007-07-25 Online:2007-07-25 Published:2011-07-25

摘要: 首先将商用活性炭样品在1%的稀硝酸中处理,然后等体积浸渍在含有5%和10%(质量分数)硝酸钴、硝酸镍或硝酸铜的水溶液中,并在100 ℃干燥至恒重,最后将样品在Ar气氛中于400 ℃焙烧3 h. 采用X射线衍射、N2吸附和红外光谱等分析手段对不同固体样品进行了表征,并考察了其对异丙醇催化转化和25~45 ℃时过氧化氢催化分解的活性. 结果表明,掺杂5%或10%的过渡金属氧化物后,活性炭样品中含有结晶度很差的CoO, Co3O4, NiO, Cu2O和CuO相的纳米晶. 金属氧化物预处理使活性炭的BET比表面积略有增加. 这些固体样品主要用作脱氢催化剂,其选择性均高于90%. 在225 ℃时,经5%氧化钴、氧化镍和氧化铜处理的活性炭的催化活性比硝酸处理的活性炭分别提高了6%, 24.6%和40.6%. 少量CoO处理后的商用活性炭对H2O2催化分解活性的提高是由参与该催化反应的活性位浓度的显著增加而引起的,该处理过程并没有改变H2O2催化分解的机理.

关键词: 活性炭, 过渡金属阳离子, 掺杂, 异丙醇转化, 过氧化氢分解

Abstract: A commercial activated carbon sample was treated with dilute nitric acid (1%) followed by impregnation with 5% and 10% cobalt, nickel, or copper nitrates, which were dissolved in the minimum amounts of distilled water sufficient to cover the surfaces of activated carbon granules followed by drying at 100 ℃ till weights became constant. The transition metal ions-treated samples were heated at 400 ℃ in a flow of argon for 3 h. The analytical tools for characterization of different solids wereX-raydiffraction, nitrogen adsorption at-196℃, infrared spectroscopy, catalytic conversion of iso-propanol, and catalytic decomposition of H2O2 at 25-45 ℃. The results revealed that the activated carbon treated with 5% and 10% transition metal oxides heated at 400 ℃ in a argon flow consisted of a mixture of very poor crystalline CoO, Co3O4, NiO, Cu2O, and CuO phases of nano-crystalline nature. The treatment of activated carbon with cobalt, copper, or nickel oxide led to a small increase in its BET surface area. All solids investigated acted mainly as dehydrogenation catalysts with selectivities above 90%. The percentage increase in the catalytic activity, measured at 225 ℃, due to the treatment with 5% transition metal oxide attained 6%, 24.6%, and 40.6% for cobalt, nickel, and copper oxides, respectively. The observed measurable increase in the catalytic activity of the commercial activated carbon system treated with small amounts of CoO in the catalysis of H2O2 decomposition can be considered as a consequence of the significant increase in the concentration of catalytically active sites taking part in the catalysis of H2O2 decomposition, but it did not modify the mechanism of the catalytic decomposition.

Key words: activated carbon, transition metal cation, doping, iso-propanol conversion, hydrogen peroxide decomposition