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不同晶相结构二氧化锰催化完全氧化乙醇
  • ISSN号:1000-6818
  • 期刊名称:《物理化学学报》
  • 时间:0
  • 分类:O643[理学—物理化学;理学—化学]
  • 作者机构:[1]中国科学院生态环境研究中心大气污染控制中心,环境模拟与污染控制国家联合重点实验室,北京100085
  • 相关基金:国家自然科学基金(21422706)及国家高技术研究发展计划项目(863)(2012AA062702)资助
中文摘要:

采用水热合成法制备了α-MnO2、β-MnO2、γ-MnO2和δ-MnO2催化剂,运用N2吸脱附实验、X射线衍射(XRD)、X射线光电子能谱(XPS)和H2程序升温还原(H2-TPR)等方法对催化剂进行了表征,并将催化剂用于催化完全氧化乙醇反应中,考察了不同晶型MnO2催化剂催化氧化乙醇活性的差异,探讨了催化剂晶型结构与催化氧化活性的关联.结果表明,不同晶型的MnO2催化剂催化氧化乙醇活性差异显著,活性顺序为α-MnO2〉δ-MnO2〉γ-MnO2〉β-MnO2.系列表征结果显示,晶体结晶度和比表面积不是影响不同晶型MnO2催化剂活性的主要原因,α-MnO2催化剂具有的较高晶格氧浓度和较高的可还原性是其具有良好催化氧化乙醇活性的关键因素.

英文摘要:

α-MnO2,β-MnO2,γ-MnO2, andδ-MnO2 catalysts were synthesized by hydrothermal methods, and their catalytic performances towards the oxidation of ethanol were evaluated in detail. The as-synthesized MnO2 catalysts were characterized by N2 adsorption-desorption measurements, X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and H2 temperature-programmed reduction (H2-TPR). Theα-MnO2 catalyst showed the best activity of the catalysts tested for the combustion of ethanol and the trend in the activity of different MnO2 catalysts towards the oxidation of ethanol was of the orderα-MnO2〉δ-MnO2〉γ-MnO2〉β-MnO2. The effect of the crystal phase structure on the activity of the MnO2 catalysts was investigated. The XRD results showed that there were differences in the crystal inities of theα-,β-,γ-,δ-MnO2 catalysts, but these differences did not have a significant effect on their catalytic performances towards the oxidation of ethanol. The BET surface areas of theα-,β-,γ-,δ-MnO2 catalysts exhibited similar tendencies to their ethanol oxidation activities, although the results of standardization calculations showed that the surface area was not the main factor affecting their catalytical activities. The XPS results showed that the lattice oxygen concentration played an important role in defining the catalytic performance of the MnO2. The α-MnO2 catalyst showed the best reducibility of al of the MnO2 catalysts tested, as determined by H2-TPR. The excel ent performance ofα-MnO2 was attributed to its higher lattice oxygen concentration and reducibility, which were identified as the main factors affecting the activity of the MnO2 towards the complete oxidation of ethanol.

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期刊信息
  • 《物理化学学报》
  • 中国科技核心期刊
  • 主管单位:中国科学技术协会
  • 主办单位:北京大学化学与分子工程学院承办
  • 主编:刘忠范
  • 地址:北京大学化学楼
  • 邮编:100871
  • 邮箱:whxb@pku.edu.cn
  • 电话:010-62751724
  • 国际标准刊号:ISSN:1000-6818
  • 国内统一刊号:ISSN:11-1892/O6
  • 邮发代号:82-163
  • 获奖情况:
  • 中文核心期刊
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国科学引文索引(扩展库),英国科学文摘数据库,日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:24781