文章摘要
王冠龙,毕晨曦,陈硕,全燮,于洪涛.氮掺杂多孔碳包覆钴金属催化去除有机污染物[J].,2018,58(4):331-341
氮掺杂多孔碳包覆钴金属催化去除有机污染物
Encapsulation of Co metal by nitrogen doped porous carbon for catalytic removal of organic pollutants
  
DOI:10.7511/dllgxb201804001
中文关键词: 过硫酸氢盐(PMS)  硫酸根自由基  氮掺杂多孔碳  核壳催化剂  苯酚降解
英文关键词: peroxymonosulfate(PMS)  sulfate radical  nitrogen doped porous carbon  core-shell catalyst  phenol degradation
基金项目:国家自然科学基金资助项目(重大项目:21590813);高等学校学科创新引智计划资助项目(B13012).
作者单位
王冠龙,毕晨曦,陈硕,全燮,于洪涛  
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中文摘要:
      活化过硫酸氢盐(PMS)产生具有强氧化能力的硫酸根自由基(SO·-4)的高级氧化技术在有机污染物降解方面正受到越来越多的关注.选择ZIF-67为前驱体通过两步热处理构建氮掺杂多孔碳包覆钴金属的核壳催化剂(Co@NPC),并通过改变碳化温度调控多孔碳壳的结构与组成,研究多孔碳结构组成对催化性能的影响.实验结果表明,随着碳化温度的升高,介孔孔容与碳壳厚度逐渐增大,催化剂的性能随着介孔孔容与碳壳厚度比值的增加而显著提高.850 ℃碳化的Co@NPC催化降解苯酚的动力学常数是多相催化剂四氧化三钴的110.8倍,甚至是之前报道过最优的PMS催化剂均相钴离子的4.6倍.此外,当包覆的碳层数大于3时,Co@NPC表现出良好稳定性,钴溶出明显减少.碳壳的介孔孔容与厚度是影响PMS活化的重要因素,Co@NPC的催化性能还受到石墨氮含量的影响.
英文摘要:
      Sulfate radical (SO·-4), which is usually obtained by peroxymonosulfate (PMS) activation, has attracted much interest in the research of organic pollutant degradation for its high oxidative capability. Herein, a Co@nitrogen doped porous carbon (Co@NPC) core-shell catalyst is prepared using ZIF-67 as the precursor by two-step heating treatment. Different carbonization temperatures are chosen to tune the structure and composition of carbon shell, and its relationship with catalytic performance is investigated. The results show that the mesopore volume and the carbon shell thickness increase gradually with the increase of carbonization temperature, while the catalytic performance is enhanced with the increasing ratio of mesopore volume to carbon shell thickness. The Co@NPC carbonized at 850 ℃ performs best for phenol degradation, whose kinetic constant for phenol degradation is 110.8 times higher than that of heterogeneous Co3O4 and even 4.6 times higher than that of the reported optimum homogeneous Co2+ for PMS activation. Moreover, the Co@NPC displays good stability and obvious reduction of Co leaching when the number of carbon layer is higher than 3. The mesopore volume and thickness of carbon shell play significant roles in the PMS activation, while the content of graphitic N could also influence the catalytic performance.
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