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摘要
以Hollandite型氧化物Pb2-xMn8O16为载体,NaBH4、甲醛和乙二醇为还原剂,采用液相沉积还原法制备了3种载Pd催化剂,并利用X射线衍射(XRD)、透射电子显微镜(TEM)、X射线光电子能谱(XPS)等技术对催化剂进行表征,分析了不同还原剂对催化剂微观结构、氧化还原性质及其在苯酚氧化羰基化反应中催化性能的影响。实验结果表明,NaBH4的强还原性破坏了载体Pb2-xMn8O16的结构;与甲醛相比,以乙二醇为还原剂所得的纳米钯粒子在载体上的分布更加均匀,Pd粒子的平均尺寸为4.1 nm。其中采用乙二醇为还原剂制备的Pd/Pb2-xMn8O16催化合成碳酸二苯酯的收率最高,达15.6%。
Abstract
Three kinds of palladium-loading catalysts are prepared through liquid-phase deposition reduction process with hollandite-type Pb2-xMn8O16 oxides as supporter and with ethylene glycol,formaldehyde and NaBH4 as reductant,respectively.The samples are characterized by X-ray diffraction (XRD),transmission electron microscopy (TEM),and X-ray photoelectron spectroscopy (XPS) techniques.Effects of the reductant on catalysts' micro-structures,redox properties and catalytic performances in oxidative carbonylation of phenol are analyzed.The experimental results prove that the structure of Pb2-xMn8O16 is destroyed when NaBH4 is used as the reductant.The nano-palladium particles of the catalyst that is prepared with ethylene glycol as the reductant distribute more uniformly on the supporter than that of the catalyst prepared with formaldehyde as the reductant.The average size of Pd particles is 4.1 nm in the ethylene glycol-reduced catalyst.Among three kinds of prepared catalysts,the ethylene glycol-reduced catalyst can obtain the highest yield of diphenyl carbonate,as high as 15.6%.
关键词
还原剂
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氧化羰基化
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氧空位
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钯催化剂
Key words
reductant
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oxidative carbonylation
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oxygen vacancy
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Pd catalyst
Author summay
白航(1992-),男,硕士,主要研究方向为工业催化,497956599@qq.com
还原剂对Pd/Pb2-xMn8O16催化剂微观结构与催化性能的影响[J].
现代化工, 2018, 38(7): 112-115,117 DOI:10.16606/j.cnki.issn0253-4320.2018.07.025