四硝基酞菁铝的合成及其催化活性研究
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摘要
由于各种燃油的使用,空气中的硫氧化物逐渐增多,要降低空气中的硫氧化物,就要降低燃油中的含硫化合物。合成了四硝基酞菁铝配合物,利用元素分析、红外光谱以及紫外-可见光谱确定了它的结构,然后以四硝基酞菁铝作为脱硫催化剂,测定了它在去除乙硫醇时的催化活性。结果表明:在四硝基酞菁铝的作用下,乙硫醇的硫氧化物去除率达到了88%,这种状况却只能持续到270min。和四羧基酞菁铝比较,由于硝基是吸电子基团,它降低了酞菁环上的电子云密度,不利于电子的转移,导致催化活性下降。
Due to the use of various fuels,sulfur oxides in the air gradually increased. In order to reduce the sulfur oxides in the air,so that to reduce sulfur compounds in the fuel. Aluminum tetranitrophthalocyanine complexes were synthesized by elemental analysis,infrared spectroscopy and ultraviolet visible spectroscopy to determine its structure,and then to the Aluminum tetranitrophthalocyanine as desulfurization catalyst,determined its catalytic activity in ethylene removal the results show that the thiol Aluminum tetranitrophthalocyanine under the effect of ethyl mercaptan removal rate reached 88%,this situation can last up to 270 min. Compared with Aluminum tetranitrophthalocyanine,the nitro group is an electron of withdrawing group,which reduces the electron cloud density on the phthalocyanine ring,which is unfavorable to the electron transfer and leads to the decrease of the catalytic activity.
Due to the use of various fuels,sulfur oxides in the air gradually increased. In order to reduce the sulfur oxides in the air,so that to reduce sulfur compounds in the fuel. Aluminum tetranitrophthalocyanine complexes were synthesized by elemental analysis,infrared spectroscopy and ultraviolet visible spectroscopy to determine its structure,and then to the Aluminum tetranitrophthalocyanine as desulfurization catalyst,determined its catalytic activity in ethylene removal the results show that the thiol Aluminum tetranitrophthalocyanine under the effect of ethyl mercaptan removal rate reached 88%,this situation can last up to 270 min. Compared with Aluminum tetranitrophthalocyanine,the nitro group is an electron of withdrawing group,which reduces the electron cloud density on the phthalocyanine ring,which is unfavorable to the electron transfer and leads to the decrease of the catalytic activity.
引文
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[2]J.K.Joseph,S.L.Jain,B.Sain.Covalently Anchored Polymer Immobilized Co(II)Phthalocyanine as Efficient Catalyst for Oxidation of Mercaptans Using Molecular Oxygen as Oxidant[J].Ind.Eng.Chem.Res,2010,49:6674-6677.
[3]Meryem Camur,Ali Rlza Ozkaya,Mustafa Bulut.Novel Phthalo-cyanines Bearing Four 4-Phenyloxyacetic Acid Functionalities[J].Polyhedron,2007,26(12):2638-2646.
[4]Shan Jin,Gongzhen Cheng,George Z.Tuning the Maximum Absorption Wavelengths of Phthalocyanine Derivatives[J].J.Porphyrins Phthalocyanines,2005(9):32-39.
[5]张焕玲.“888”型催化剂在煤气脱硫装置上的应用[J].山东石油化工,2006(1):36-38.
[6]董国孝,李纪生,庄瑞舫.四羧基酞菁配合物修饰电极对分子氧的电还原[J].分子催化,1996,10(1):19-24.
[7]Wesley M.Sharman,Johan E.van Lier.A New Procedure for the Synthesis of Water-soluble Tricationic and Anionic Phthalo-cyanines[J].J.Porphyrins Phthalocyanines,2005(9):651-658.
[8]John Mack,Martin J.Stillman.Assignment of the Optical Spectra of Metal Phthalocyanines Through Spectral Band Deconvolution Analysis and ZINDO Calculations[J].Coordin.Chem.Rev.,2001,219:993-1032.
[9]Meryem N.Yarasir,Mehmet Kandaz,B.Filiz Senkal,et al.Metal-ion Sensing and Aggregation Studies on Reactive Phthalocyanines Bearing Soft-metal Receptor Moieties,Synthesis,Spectroscopy and Electrochemistry[J].Polyhedron,2007,26,5235-5242.