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纳米CeO2催化氧化甲苯的形貌效应研究
引用本文:何丽芳,廖银念,陈礼敏,付名利,吴军良,黄碧纯,叶代启. 纳米CeO2催化氧化甲苯的形貌效应研究[J]. 环境科学学报, 2013, 33(9): 2412-2421
作者姓名:何丽芳  廖银念  陈礼敏  付名利  吴军良  黄碧纯  叶代启
作者单位:1. 华南理工大学环境与能源学院,广州,510006
2. 华南理工大学环境与能源学院,广州,510006;新疆大学化学化工学院,乌鲁木齐,830046
3. 华南理工大学环境与能源学院,广州,510006;大气环境与污染控制广东省重点实验室,广州,510006;广东高校大气污染控制工程研究中心,广州510006
基金项目:国家自然科学基金项目,中央高校基本科研业务费专项资金,the National Natural Science Foundation of China,the Research Business Expenses of Central High University
摘    要:采用水热法合成CeO2纳米棒、纳米颗粒和纳米立方体,利用XRD、BET-N2、TEM/HRTEM、Raman、O2-TPD和H2-TPR等表征手段进行表征,并利用连续流固定床反应法研究各催化剂对甲苯的催化氧化性能.结果表明,CeO2纳米棒因具有高比表面积和细颗粒尺寸,且表面主要暴露高活性的{100}/{110}晶面,拥有更多的氧空位和高活性氧物种,因此,催化活性最高,CeO2纳米颗粒次之,立方体最低.原位红外甲苯催化氧化机理分析进一步表明,CeO2纳米颗粒和纳米立方体上生成的羧酸盐物质难以进一步深度氧化,而纳米棒能在贫氧和低温条件下诱导甲苯的完全氧化和产物脱附,使甲苯得以快速降解.

关 键 词:纳米CeO2  甲苯  催化氧化  形貌效应
收稿时间:2013-01-06
修稿时间:2013-01-30

Shape effect of ceria nanocrystals with various morphologies on toluene catalytic oxidation
HE Lifang,LIAO Yinnian,CHEN Limin,FU Mingli,WU Junliang,HUANG Bichun and YE Daiqi. Shape effect of ceria nanocrystals with various morphologies on toluene catalytic oxidation[J]. Acta Scientiae Circumstantiae, 2013, 33(9): 2412-2421
Authors:HE Lifang  LIAO Yinnian  CHEN Limin  FU Mingli  WU Junliang  HUANG Bichun  YE Daiqi
Affiliation:College of Environment and Energy, South China University of Technology, Guangzhou 510006;1. College of Environment and Energy, South China University of Technology, Guangzhou 510006;2. College of Chemistry and Chemical Engineering, Xinjiang University, Urumqi 830046;College of Environment and Energy, South China University of Technology, Guangzhou 510006;College of Environment and Energy, South China University of Technology, Guangzhou 510006;College of Environment and Energy, South China University of Technology, Guangzhou 510006;College of Environment and Energy, South China University of Technology, Guangzhou 510006;1. College of Environment and Energy, South China University of Technology, Guangzhou 510006;2. Guangdong Provincial Key Laboratory of Atmospheric Environment and Pollution Control, Guangzhou 510006;3. Guangdong High Education Engineering Technology Research Center for Air Pollution Control, Guangzhou 510006
Abstract:Ceria nanorods, nanoparticles and nanocubes catalysts were fabricated by a simple hydrothermal method, and their catalytic performances were evaluated for toluene oxidation in a continuous fixed bed reactor. The properties of the synthesized catalysts were characterized by X-ray diffraction (XRD), N2 adsorption (BET), transmission electron microscopy/high-resolution transmission electron microscopy (TEM/HRTEM), Raman, oxygen temperature-programmed desorption (O2-TPD) and hydrogen temperature-programmed reduction (H2-TPR). The results indicated that ceria nanorods showed greater surface area, smaller crystallite size and more reactive {100} and {110} planes exposure on the surface, giving more oxygen vacancies and reactive oxygen species compared to Ceria nanoparticles and nanocubes., These led to the highest catalytic activity towards toluene oxidation. Furthermore, the mechanism of adsorption-oxidation of toluene via in-situ IR was investigated. The results indicated that it was difficult to further oxidize the intermediates and carboxylate that were generated on ceria nanoparticles or nanocubes. In comparison, it was easier to achieve complete oxidation of toluene and product desorption on nanorods in the lean oxygen at low temperature, favoring the rapid degradation of toluene.
Keywords:ceria nanocrystals  toluene  catalytic oxidation  shape effect
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