Surface modification of CeO2 nanoflakes by low temperature plasma treatment to enhance imine yield: Influences of different plasma atmospheres

Surface modification of CeO2 nanoflakes by low temperature plasma treatment to enhance imine yield: Influences of different plasma atmospheres
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低温等离子体处理CeO2纳米片表面改性提高亚胺产率:不同等离子体气氛的影响

DOI:
10.1016/j.apsusc.2018.05.135
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发表时间:
2018-10
影响因子:
6.7
通讯作者:
Xijiang Chang
Xijiang Chang
中科院分区:
材料科学1区
文献类型:
--
作者:
Jingxia Yang;Huihui Ding;Zhu Zhu;Qiuhe Wang;Jinjie Wang;Jingli Xu;Xijiang Chang

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在不同气氛(Ar、H2、O2和NH3的组合)下对溶剂热合成的CeO 2纳米片进行等离子体处理,并进一步用于亚胺合成。等离子体处理可以改善表面氧空位的量、Ce 3+比率和过氧阴离子O22−比率。这三个参数对CeO 2催化亚胺转化反应的催化能力都有不同程度的影响。以H2和O2为工作气体的等离子体能显著提高过氧化阴离子O22-的比例(从3.14%提高到40%左右),而以Ar + H2和Ar + NH3为工作气体的等离子体能显著提高Ce 3+的比例(约28.54%)和表面氧空位。采用Ar + H2混合气体作为等离子体气氛时,亚胺合成反应速率可提高到原始CeO 2的75%。CeO 2表面氧空位的数量是亚胺转化的最重要参数。催化活性的提高主要是由于表面氧空位和Ce 3+比例的提高,而过氧阴离子O22−比例的提高则是催化活性提高的主要原因。
Solvothermal synthesized CeO2nanoflakes were plasma treated under different atmospheres (combination of Ar, H2, O2and NH3), and further used for imine synthesis. The plasma processing can improve the amount of surface oxygen vacancies, Ce3+ratio, and the peroxy anions O22−ratio. All the three parameters can influence the CeO2catalytic ability of imine conversion to different extent. The plasma with working gas of H2and/or O2can increase the peroxy anions O22−ratio greatly (from 3.14% to about 40%), while the reducing condition (Ar + H2and Ar + NH3as working gas) can significantly improve the Ce3+ratio (∼28.54%) and the surface oxygen vacancies. The reaction rate of imine synthesis can be improved up to 75% of the pristine CeO2when Ar + H2mixture gas was used as the plasma atmosphere. The amount of CeO2surface oxygen vacancies is the most important parameter for imine conversion. The enhancement of catalytic ability can be mainly attributed to the improved surface oxygen vacancies and the Ce3+ratio, and slightly to the rising of peroxy anions O22−ratio, although the value of the last parameter increased most.
表面氧空位占主导地位的CeO 2 作为亚胺合成的有效催化剂:不同铈前驱体的影响
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