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聚乙二醇辅助下的La-Co-O 复合氧化物合成及其对苯的完全氧化性能研究
引用本文:魏笑峰,李达林,肖益鸿,蔡国辉,戴武,谢增鸿,魏可镁.聚乙二醇辅助下的La-Co-O 复合氧化物合成及其对苯的完全氧化性能研究[J].光谱学与光谱分析,2016,36(9):3062-3067.
作者姓名:魏笑峰  李达林  肖益鸿  蔡国辉  戴武  谢增鸿  魏可镁
作者单位:1. 福州大学化肥催化剂国家工程研究中心, 福建 福州 350002
2. 福州大学化学学院,福建 福州 350108
基金项目:National Science Foundation(40976071 and 21377024),Key S&T Project of Fujian Province(2014H6015),the Pro-gram from the Fujian Education Department(JA12023)
摘    要:以聚乙二醇(PEG)作为分散剂,采用共沉淀法合成La-Co-O复合氧化物,考察添加不同分子量的PEG (0, 2 000, 6 000, 20 000 g·mol-1) 对复合氧化物的物化性质及苯完全氧化性能的影响。采用N2物理吸附、XRD、SEM、H2-TPR、O2-TPD和XPS进行催化剂表征。苯完全氧化反应结果显示催化剂活性顺序为LCO-PEG6000>LCO>LCO-PG20000>LCO-PG2000, LCO-PEG6000催化剂在383 ℃时对苯的转化率达到99%,比LCO低126 ℃。N2物理吸附实验表明所制备的样品的SBET均为9~10 m2·g-1。XRD分析显示合成的催化剂均为LaCoO3钙钛矿主相伴生少量La2O3和Co3O4杂相,但添加PEG有利于钙钛矿主相的形成。尤其是添加PEG6000有效地抑制了催化剂颗粒的团聚,合成的样品颗粒均匀且尺寸最小。H2-TPR和O2-TPD结果表明该催化剂具有更高的还原性能和晶格氧迁移能力,同时XPS分析显示表面活性Co3+含量最高,这些性质使其具有最高的催化氧化活性。

关 键 词:复合氧化物  LaCoO3  聚乙二醇  共沉淀法  催化燃烧  苯完全氧化    
收稿时间:2015-04-17

Synthesis of La-Co-O Mixed Oxides via Polyethylene Glycol-Assisted Co-Precipitation Method for Total Oxidation of Benzene
WEI Xiao-feng,LI Da-lin,XIAO Yi-hong,CAI Guo-hui,DAI Wu,XIE Zeng-hong,WEI Ke-mei.Synthesis of La-Co-O Mixed Oxides via Polyethylene Glycol-Assisted Co-Precipitation Method for Total Oxidation of Benzene[J].Spectroscopy and Spectral Analysis,2016,36(9):3062-3067.
Authors:WEI Xiao-feng  LI Da-lin  XIAO Yi-hong  CAI Guo-hui  DAI Wu  XIE Zeng-hong  WEI Ke-mei
Institution:1. National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, China2. Faculty of Chemistry, Fuzhou University, Fuzhou 350108, China
Abstract:La-Co-O mixed oxides (LCO)were prepared by co-precipitation method with the presence of poly-ethylene glycol (PEG)as dispersant.The influence of adding different molecular weight of PEG (0,2 000, 6 000,20 000 g·mol-1 )on the physicochemical and catalytic properties of La-Co-O mixed oxides for total ox-idation of benzene was investigated.The samples were characterized by means of N2 physical adsorption,X-ray diffraction (XRD),scanning electron microscopy (SEM),temperature-programmed reduction by H2 (H2-TPR),temperature-programmed desorption of O2 (O2-TPD),and X-ray photoelectron spectroscopy (XPS). The order of catalytic activity was found to be LCO-PEG6000>LCO>LCO-PG20000>LCO-PG2000.Partic-ularly,LCO-PEG6000 exhibited benzene conversion of 99% at temperature as low as 383 ℃,which was 126℃ lower than that of LCO.The characterization result reveals that all samples had a BET surface area of about 9~10 m2 ·g-1 .The XRD result shows that on all samples LaCoO3 perovskite was mainly formed together with a small amount of La2 O3 and Co3 O4 .The addition of PEG was favorable for the formation of LaCoO3 per-ovskite.Particularly,the addition of PEG-6000 effectively suppressed the agglomeration of LaCoO3 perovs-kite,giving rise to small and uniform particles as observed by SEM.Moreover,the results of H2-TPR and O2-TPD indicate that the obtained La-Co-O mixed oxides showed higher reducibility and lattice oxygen mobility, and the Co 2p XPS analysis suggests that more surface Co3+ active species were presented by the addition of PEG-6000.These properties are thought to contribute to the high activity in benzene total oxidation.
Keywords:Mixed oxides  LaCoO3  Polyethylene glycol  Co-precipitation  Catalytic combustion  Benzene total oxidation
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