郭一曼,马莉娟,陈小梅,袁霞.MCF介孔分子筛负载Co催化环己基过氧化氢分解[J].分子催化,2019,33(2):140-148
MCF介孔分子筛负载Co催化环己基过氧化氢分解
MCF Mesoporous Molecular Sieve Supported Co Catalyzed Decomposition of Cyclohexyl Hydroperoxide
投稿时间:2019-01-03  修订日期:2019-03-03
DOI:
中文关键词:    MCF  环己基过氧化氢  分解
英文关键词:cobalt  MCF  cyclohexyl hydroperoxide  decomposition
基金项目:国家自然科学基金资助项目(No.21776237);"环境友好与资源高效利用化工新技术"湖南省高校2011协同创新中心资助项目
作者单位E-mail
郭一曼 湘潭大学 化工学院, 湖南 湘潭 411105  
马莉娟 湘潭大学 化工学院, 湖南 湘潭 411105  
陈小梅 湘潭大学 化工学院, 湖南 湘潭 411105  
袁霞 湘潭大学 化工学院, 湖南 湘潭 411105 yuanxia@xtu.edu.cn 
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中文摘要:
      以P123为模板剂,1,3,5-三甲苯(TMB)为扩孔剂,正硅酸乙酯(TEOS)为硅源,六水硝酸钴为钴源,在酸性条件下原位合成XCo-MCF (X=4%,8%,10%,20%)介孔分子筛.采用FT-IR、UV-Vis、氮气物理吸附、XRD、XPS、H2-TPR等手段对XCo-MCF的结构进行表征,并在环己基过氧化氢(CHHP)分解反应中进行了催化性能评价.UV-Vis、XPS和XRD等表征结果表明,XCo-MCF中钴主要以Co3O4的形式存在.以CHHP含量为7.2%(重量百分比)的环己烷氧化液为原料,XCo-MCF催化CHHP分解,在80℃反应90 min,CHHP分解转化率均在90%以上,其中8% Co-MCF为催化剂时,CHHP转化率达到95.7%,环己醇和环己酮选择性分别为77.5%和53.4%.经过4次回收重复使用后,催化剂仍能够保持较高的活性,ICP表征表明各催化剂活性组分均存在一定程度的流失,负载量达到20%时,活性组分的流失速率得到明显抑制.
英文摘要:
      Cobalt-containing mesoporous molecular sieves XCo-MCF (X=4%, 8%, 10%, 20%) were synthesized in situ under acidic conditions using P123 as template, 1,3,5-trimethylbenzene (TMB) as pore-enlarging agent, tetraethyil orthosilicate (TEOS) as silicon source, and Co(NO3)2·6H2O as cobalt source. The structures of XCo-MCF were characterized by the methods of FT-IR, UV-Vis, N2 adsorption/desorption, XRD, XPS and H2-TPR. The catalytic performance of the obtained samples was evaluated in decomposition of cyclohexyl hydroperoxide (CHHP). The characterization results of UV-Vis, XPS and XRD indicated that cobalt in XCo-MCF mainly existed in the form of Co3O4. The cyclohexane oxidation solution with CHHP content of 7.2%(Weight percentage) was used as raw material, the decomposition of CHHP was catalyzed by XCo-MCF at 80℃ for 90 min. The conversion of CHHP is above 90%. 8%Co-MCF showed the better catalytic performance with a conversion of 95.7% and the selectivity of cyclohexanol 77.5% and cyclohexanone 53.4%. After four times of repeated uses, the catalysts still maintained high activity. The ICP characterization results showed that the active components of each catalyst were lost to some extent. When the loading amount of Cobalt reached 20%, the loss rate of the active components was significantly inhibited.
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