铂纳米颗粒增强MnO2纳米棒对CO和挥发性有机化合物的氧化活性

doi:10.3866/PKU.WHXB201112082

物理化学学报 >> 2012, Vol. 28 >> Issue (02): 437-444.doi: 10.3866/PKU.WHXB201112082

铂纳米颗粒增强MnO₂纳米棒对CO和挥发性有机化合物的氧化活性

吴小琴^1,2, 宗瑞隆¹, 朱永法¹

1. 清华大学化学系, 北京 100084;
2. 南昌航空大学环境与化学工程学院, 南昌 330063

收稿日期:2011-09-29 修回日期:2011-12-01 发布日期:2012-01-11
通讯作者: 吴小琴, 朱永法 E-mail:zhuyf@tsinghua.edu.cn; wxq968@sina.com
基金资助:
国家自然科学基金(20925725), 国家重点基础研究发展规划项目(973) (2007CB613303)和江西省教育厅科技项目(GJJ11507)资助

Enhanced MnO₂ Nanorods to CO and Volatile Organic Compounds Oxidative Activity by Platinum Nanoparticles

WU Xiao-Qin^1,2, ZONG Rui-Long¹, ZHU Yong-Fa¹

1. Department of Chemistry, Tsinghua University, Beijing 100084, P. R. China;
2. College of Environmental and Chemical Engineering, Nanchang Hang Kong University, Nanchang 330063, P. R .China

Received:2011-09-29 Revised:2011-12-01 Published:2012-01-11
Contact: WU Xiao-Qin, ZHU Yong-Fa E-mail:zhuyf@tsinghua.edu.cn; wxq968@sina.com
Supported by:
The project was supported by the National Natural Science Foundation of China (20925725), National Key Basic Research Program of China (973) (2007CB613303), and Jiangxi Provincial Department of Education Technology Project, China (GJJ11507).

摘要/Abstract

摘要： 通过水热法合成了纯相的α-MnO₂和δ-MnO₂纳米棒, 并利用溶胶固定化工艺制备了负载铂纳米颗粒的Pt/MnO₂材料. 通过透射电镜(TEM), X射线粉末衍射(XRD), 扫描电镜(SEM), X射线光电子能谱(XPS), N₂吸附-脱附和H₂程序升温还原(H₂-TPR)技术研究了样品的微观结构和吸附活性位, 探查了CO和挥发性有机化合物(VOCs)(苯和甲苯)在催化剂上的催化发光(CTL)性质. 结果表明: 铂颗粒在α-MnO₂和δ-MnO₂载体上以高分散状态存在, 负载过程不会影响α-MnO₂纳米棒的晶相结构, 但会导致δ-MnO₂纳米棒产生结构变化. 经XPS证实不是Pt 与其发生了反应. α-和δ-MnO₂纳米棒对CO、苯和甲苯的催化氧化都具有很高的活性, δ-MnO₂的活性略高于α-MnO₂相. 虽然N₂吸附-脱附实验结果证实Pt 负载会导致MnO₂纳米棒比表面积的下降, 但H₂-TPR 结果显示Pt 和MnO₂之间会产生强烈的相互作用, 显著增强其催化活性, 且Pt/δ-MnO₂活性高于Pt/α-MnO₂. 催化氧化发光研究表明, 这四种催化剂活性顺序是α-MnO₂≤δ-MnO₂ < Pt/α-MnO₂ < Pt/δ-MnO₂, 与H₂-TPR 结果一致.铂的负载可以显著增强α-MnO₂和δ-MnO₂纳米棒对CO、苯和甲苯催化氧化的活性.

关键词: 催化活性, MnO₂纳米棒, Pt纳米颗粒, 催化发光, CO, 苯, 甲苯

Abstract: Pure-phase α-MnO₂ and δ-MnO₂ nanorods were synthesized through an easy solution-based hydrothermal method. Platinum nanoparticles supported by the obtained MnO₂ nanorods were prepared by the colloid deposition process. The microstructure and adsorption activity of the obtained catalysts were researched by different techniques such as transmission electron microscopy (TEM), powder X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), N₂ adsorption-desorption measurements, and H₂ temperature-programmed reduction (H₂-TPR). The cataluminescence (CTL) properties of CO and volatile organic compounds (VOCs), such as benzene and toluene, on the resultant catalysts were explored. The results showed that the platinum nanoparticles were well distributed in α-MnO₂ and δ-MnO₂. In addition, the Pt load process does not affect the crystal phase structure of the α-MnO₂ nanorods, but can generate structural changes in the δ-MnO₂ nanorods. The phase transformation did not the result of the reaction between the δ-MnO₂ nanorods and Pt as shown in the XPS study. The α-MnO₂ and δ-MnO₂ nanorods showed a high catalytic oxidative activity toward CO, benzene, and toluene, and δ-MnO₂ showed a higher activity than the α-MnO₂ phase. Although, the Pt load led to a decrease in the surface area of the MnO₂ nanorods which was confirmed by the N₂ adsorption-desorption measurements, but the H₂-TPR results showed that the interaction between Pt and MnO₂ was intense, which significantly enhanced its catalytic activity. The Pt/δ-MnO₂ nanorods exhibited a higher activity than Pt/α-MnO₂. CTL research showed that the activities of the four catalysts increased in the order of α-MnO₂≤ δ-MnO₂ < Pt/α-MnO₂ < Pt/δ-MnO₂, and the H₂-TPR results were consistent. Pt loading significantly enhanced the catalytic oxidative activity of α-MnO₂ and δ-MnO₂ nanorods to CO, benzene, and toluene.

Key words: Catalytic activity, MnO₂ nanorod, Pt nanoparticle, Cataluminescence, CO, Benzene, Toluene

MSC2000:

O643

吴小琴, 宗瑞隆, 朱永法. 铂纳米颗粒增强MnO₂纳米棒对CO和挥发性有机化合物的氧化活性[J]. 物理化学学报, 2012, 28(02): 437-444.

WU Xiao-Qin, ZONG Rui-Long, ZHU Yong-Fa. Enhanced MnO₂ Nanorods to CO and Volatile Organic Compounds Oxidative Activity by Platinum Nanoparticles[J]. Acta Phys. -Chim. Sin., 2012, 28(02): 437-444.

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铂纳米颗粒增强MnO₂纳米棒对CO和挥发性有机化合物的氧化活性

Enhanced MnO₂ Nanorods to CO and Volatile Organic Compounds Oxidative Activity by Platinum Nanoparticles

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