白哲,代方方,贾敏杰,刘娜,时米东.适宜氧空位诱导α-MnO2高效催化消除碳烟研究[J].分子催化,2021,35(6):529-537
适宜氧空位诱导α-MnO2高效催化消除碳烟研究
Suitable Oxygen Vacancies Induce α-MnO2 Catalyst to Efficiently Eliminate Soot
投稿时间:2021-08-13  修订日期:2021-10-07
DOI:10.16084/j.issn1001-3555.2021.06.004
中文关键词:  碳烟催化燃烧  氧空位  化学吸附氧
英文关键词:soot catalytic combustion  oxygen vacancy  chemisorption oxygen
基金项目:国家自然科学基金青年项目(21706150),陕西省自然科学基金一般项目(2019JQ-789),湘南稀贵金属化合物及其应用湖南省重点实验室(湘南学院)(2019XGJSKFJJ04)
作者单位E-mail
白哲 陕西科技大学, 陕西 西安 710021  
代方方 陕西科技大学, 陕西 西安 710021
湘南稀贵金属化合物及其应用湖南省重点实验室, 湖南 郴州 423000 
daifangfang@sust.edu.cn 
贾敏杰 陕西科技大学, 陕西 西安 710021  
刘娜 陕西科技大学, 陕西 西安 710021  
时米东 湘南稀贵金属化合物及其应用湖南省重点实验室, 湖南 郴州 423000  
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中文摘要:
      柴油机排放的碳烟颗粒对人类和自然产生了严重的威胁,开发高活性低成本的碳烟燃烧催化剂是解决这一问题的关键.我们采用不同煅烧气氛(空气、真空和氮气)成功制备了含有不同浓度氧空位的α-MnO2催化剂(记为M-Air-500,M-Va-500,M-N-500,M-N-450).M-Va-500和M-N-500催化剂在500℃煅烧时会失去过多晶格氧,导致晶相结构发生改变,出现Mn3O4相,这与XRD和HRTEM结果一致.XPS和Soot-TPR的结果说明,催化剂表面的化学吸附氧提高了催化剂的催化性能.H2-TPR结果说明适量的氧空位能够加快晶格氧的迁移,提高可移动氧物种丰度,增强催化剂的氧化能力.结合催化活性测试结果可以得出:在保持α-MnO2晶相结构的前提下,氧空位越多,催化剂表面的化学吸附氧越多,催化活性越好.
英文摘要:
      The soot particles emitted by diesel engines pose a serious threat to human beings and nature. The key to solve this problem is to develop a high activity and low cost soot combustion catalyst. In this work, α-MnO2 catalysts with different concentrations of oxygen vacancies were successfully prepared under different calcination atmospheres (named as M-Air-500, M-Va-500, M-N-500, M-N-450). M-Va-500 and M-N-500 catalysts will lose too much lattice oxygen when calcined at 500℃, and cause the crystal phase structure change, the presence of Mn3O4 phase, this is consistent with the XRD and HRTEM results. The results of XPS and Soot-TPR indicate that the catalytic performance of the catalyst was improved by chemical adsorption oxygen. The H2-TPR results show that a proper amount of oxygen vacancies can accelerate the migration of lattice oxygen, increase the abundance of movable oxygen species, and enhance the oxidation ability of the material. Combined with the catalytic activity test results, we conclude that with the concentration of oxygen vacancies increases, the amount of chemically adsorbed oxygen on the catalyst surface increases, which leads to an increase in catalytic activity. But the premise is that the catalyst crystal phase has not changed.
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