一维ZnO表面可控构建Co3Mn1纳米晶及其催化CO氧化性能
Controlled construction of Co3Mn1 nanocrystals on one-dimensional ZnO surfaces for catalytic performance of CO oxidation
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刘新月 中南民族大学, 催化转化与能源材料化学教育部重点实验室&催化材料科学湖北省重点实验室, 武汉 430074  
吕帅 中南民族大学, 催化转化与能源材料化学教育部重点实验室&催化材料科学湖北省重点实验室, 武汉 430074  
张煜华 中南民族大学, 催化转化与能源材料化学教育部重点实验室&催化材料科学湖北省重点实验室, 武汉 430074  
李金林 中南民族大学, 催化转化与能源材料化学教育部重点实验室&催化材料科学湖北省重点实验室, 武汉 430074  
王立 中南民族大学, 催化转化与能源材料化学教育部重点实验室&催化材料科学湖北省重点实验室, 武汉 430074 li.wang@scuec.edu.cn 
摘要: 利用热分解法制备了结构明确的负载型纳米晶催化剂。在纳米晶成核和生长过程中加入一维ZnO纳米棒作为晶种,调控不同组分的纳米晶在ZnO纳米棒表面均匀生长,从而获得了结构明确的MnO/ZnO、Co3O4/ZnO、Co3Mn1/ZnO催化剂。透射电子显微镜(TEM)与X射线粉末衍射(XRD)结果显示,不同组分纳米颗粒都均匀分散在ZnO纳米棒表面。相对于MnO/ZnO和Co3O4/ZnO催化剂,Co3Mn1/ZnO催化剂在CO氧化反应中具有最佳的催化性能。在200 L·gcat-1·h-1的气时空速下,Co3Mn1/ZnO催化剂起活温度为50℃,其T100(CO转化率达到100%时的温度)为200℃;利用X射线光电子能谱(XPS)对不同催化剂进行了分析,结果显示,Co3Mn1/ZnO催化剂的氧空位比MnO/ZnO催化剂提高了30%以上,从而使其具有较高的CO氧化催化性能。更为重要的是,Co3Mn1/ZnO复合纳米晶催化剂的活化能(39.4 kJ·mol-1)远低于其它负载型纳米晶催化剂。
关键词: CO氧化  ZnO  Co3O4  CoMn纳米晶
基金项目: 国家自然科学基金(No.22072184)资助。
Abstract: We have prepared well-defined supported nanocrystal catalysts using a thermal decomposition method. One-dimensional ZnO nanorods were used as crystalline seeds during nanocrystal nucleation and growth. The growth of nanocrystals with different components on the surface of ZnO nanorods was systematically controlled. Moreover, well-defined MnO/ZnO, Co3O4/ZnO, and Co3Mn1/ZnO catalysts were synthesized by a modified thermal decomposition approach. Transmission electron microscope (TEM) and X-ray powder diffraction (XRD) results showed that different nanocrystals were uniformly dispersed on the surface of as-synthesized ZnO nanorods. The Co3Mn1/ZnO catalyst exhibited the best catalytic performance of CO oxidation compared to the MnO/ZnO and Co3O4/ZnO catalysts. The Co3Mn1/ZnO catalyst can easily catalyze CO oxidation at a lower temperature (50℃) with sustainable durability. Moreover, the T100 (the temperature when CO conversion reached 100%) of Co3Mn1/ZnO catalyst was 200℃ at gas hourly space velocity of 200 L·gcat-1·h-1. The surface characterization of the different catalysts was performed by using X-ray photoelectron spectroscopy (XPS). The results revealed that the Co3Mn1/ZnO catalyst had approximately 30% more oxygen vacancy compared to the MnO/ZnO catalyst, resulting in a higher catalytic activity of the CO oxidation reaction. More importantly, the Co3Mn1/ZnO catalyst had a much lower apparent activation barrier (39.4 kJ·mol-1) than the other supported nanocrystal catalysts.
Keywords: CO oxidation  ZnO  Co3O4  CoMn nanocrystals
投稿时间:2022-11-18 修订日期:2023-02-13
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刘新月,吕帅,张煜华,李金林,王立.一维ZnO表面可控构建Co3Mn1纳米晶及其催化CO氧化性能[J].无机化学学报,2023,39(5):853-858.
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