CuxCo1-xAl2O4尖晶石催化合成N-乙基苯胺的研究

吕新宇, 吕正伟, 邱滔*

化工新型材料 ›› 2024, Vol. 52 ›› Issue (11) : 192 -197.

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化工新型材料 ›› 2024, Vol. 52 ›› Issue (11) : 192-197. DOI: 10.19817/j.cnki.issn1006-3536.2024.11.033
科学研究

CuxCo1-xAl2O4尖晶石催化合成N-乙基苯胺的研究

    吕新宇, 吕正伟, 邱滔*
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Synthesis and process research of N-ethylaniline catalyzed by CuxCo1-xAl2O4 spinel

  • Lv Xinyu, Lv Zhengwei, Qiu Tao
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摘要

以硝酸盐为金属源,NaOH为沉淀剂,采用共沉淀法制备CuxCo1-xAl2O4(x=1,0.75,0.5,0.25,0)系列尖晶石型催化剂。采用X射线衍射(XRD)、X射线荧光光谱仪(XRF)、X射线光电子能谱仪(XPS)、N2吸-脱附、扫描电镜(SEM)、NH3-程序升温脱附(NH3-TPD)等技术对催化剂进行表征。以乙醇作为苯胺的烷基化试剂催化合成N-乙基苯胺(N-EA),考察了催化剂元素组成、反应温度、胺醇摩尔比、质量空速、反应压力对N-EA收率的影响。结果表明:Cu0.75Co0.25Al2O4尖晶石催化合成N-EA的最优工艺条件为反应温度240℃、质量空速1.2h-1、醇胺摩尔比为2.25、反应压力3MPa,此时N-EA收率可达81.56%,选择性高达90.82%。

Abstract

CuxCo1-xAl2O4(x=1,0.75,0.5,0.25,0) series spinel catalysts were prepared by co-precipitation method using nitrate as metal source and NaOH as precipitator.The catalysts were characterized by XRD,XRF,XPS,SEM,N2 absorption-desorption and NH3-TPD.N-ethylaniline (N-EA) was synthesized using ethanol as an alkylating agent of aniline.The effects of catalyst element composition,reaction temperature,molar ratio of amine to alcohol,mass space velocity and reaction pressure on the yield of N-EA were investigated.The results showed that the N-EA yield of Cu0.75Co0.25Al2O4 was 81.56% and the selectivity was as high as 90.82% under the optimum conditions of temperature of 240℃,mass space velocity of 1.2h-1,molar ratio of alcohol to amine of 2.25 and pressure of 3MPa.

关键词

尖晶石催化剂 / 苯胺烷基化 / 固定床反应器 / N-乙基苯胺

Key words

spinel catalyst / aniline alkylation / fixed bed reactor / N-ethylaniline

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CuxCo1-xAl2O4尖晶石催化合成N-乙基苯胺的研究[J]. 化工新型材料, 2024, 52(11): 192-197 DOI:10.19817/j.cnki.issn1006-3536.2024.11.033

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参考文献

[1] Kuriakose G,Nagy J B,Nagaraju N.Structure and catalytic activity correlation of CoAlPO4 in the synthesis of N,N-biphenyl urea via alkylation of aniline using dimethyl carbonate[J].Catalysis Communications,2005,6(1):29-35.
[2] Li X N,Zhang J H,Xiang Y Z,et al.One pot synthesis of N-ethylaniline from nitrobenzene and ethanol[J].Science in China Series B:Chemistry,2008,51(3):248-256.
[3] Anand R,Khaire S S,Maheswari R,et al.N-Alkylation of aniline with ethanol over HY and dealuminated HY zeolites[J].Applied Catalysis A:General,2003,242(1):171-177.
[4] 马占玲,金东生,陶克毅.气相法合成N-乙基苯胺工艺条件和催化剂的研究[J].工业催化,2004,12(1):25-29.
[5] Mahmood M,Yousuf M A,Baig M M,et al.Spinel ferrite magnetic nanostructures at the surface of graphene sheets for visible light photocatalysis applications[J].Physica B:Condensed Matter,2018,550:317-323.
[6] Ogugua S N,Ntwaeaborwa O M,Swart H C.Luminescence,structure and insight on the inversion degree from normal to inverse spinel in a ZnAl(2-x)Fe3+xO4 system[J].Boletín de la Sociedad Espantilde;ola de Cerámica y Vidrio,2021,60(3):147-162.
[7] Jayasree S,Manikandan A,Antony S A,et al.Magneto-optical and catalytic properties of recyclable spinel NiAl2O4 nanostructures using facile combustion methods[J].Journal of Superconductivity and Novel Magnetism,2016,29:253-263.
[8] Ganesh I.A review on magnesium aluminate (MgAl2O4) spinel:synthesis,processing and applications[J].International Materials Reviews,2013,58(2):63-112.
[9] 朱文娟,高凤雨,唐晓龙,等.尖晶石型催化剂的制备及在气态污染物净化中的应用综述[J].材料导报,2020,34(3):3044-3055.
[10] 郭明星,黄均妍,刘文超.CoAl2O4催化剂对乙苯的催化性能[J].大连海事大学学报,2022,48(3):121-128.
[11] 苏玉长,赖智广,邹启凡,等.原位XRD研究合成尖晶石LiMn2O4的相变机理[J].矿冶工程,2007,27(4):87-89.
[12] Mostafa M M M,Bajafar W,Gu L,et al.Electrochemical characteristics of nanosized Cu,Ni,and Zn cobaltite spinel materials[J].Catalysts,2022,12(8):893.
[13] Tangcharoen T,Klysubun W,Jiraroj T,et al.Cation exchange in Ni-Cu-Zn aluminate spinels revealed by EXAFS[J].Journal of Solid State Chemistry,2020,292:121695.
[14] Liu Y,Kang H,Hou X,et al.Cu-Ni-Al spinel catalyzed methanol steam reforming for hydrogen production:effect of Al content[J].Journal of Fuel Chemistry and Technology,2020,48(9):1112-1121.
[15] Zeng J,Xie H,Zhang G,et al.Facile synthesis of CuCo spinel composite oxides for toluene oxidation in air[J].Ceramics International,2020,46(13):21542-21550.
[16] Feng S,Liu J,Gao B.Synergistic mechanism of Cu-Mn-Ce oxides in mesoporous ceramic base catalyst for VOCs microwave catalytic combustion[J].Chemical Engineering Journal,2022,429:132302.
[17] Duan X,Pan M,Yu F,et al.Synthesis,structure and optical properties of CoAl2O4 spinel nanocrystals[J].Journal of Alloys and Compounds,2011,509(3):1079-1083.
[18] Fierro G,Lo Jacono M,Inversi M,et al.TPR and XPS study of cobalt-copper mixed oxide catalysts:evidence of a strong Co-Cu interaction[J].Topics in Catalysis,2000,10:39-48.
[19] Tshabalala K G,Cho S H,Park J K,et al.Luminescent properties and X-ray photoelectron spectroscopy study of ZnAl2O4∶Ce3+,Tb3+ phosphor[J].Journal of alloys and compounds,2011,509(41):10115-10120.
[20] Alvar E N,Rezaei M,Alvar H N.Synthesis of mesoporous nanocrystalline MgAl2O4spinel via surfactant assisted precipitation route[J].Powder Technology,2010,198(2):275-278.
[21] Zarei M,Meshkani F,Rezaei M.Preparation of mesoporous nanocrystalline Ni-MgAl2O4 catalysts by sol-gel combustion method and its applications in dry reforming reaction[J].Advanced Powder Technology,2016,27(5):1963-1970.
[22] Zhang J,Liu X,Deng L,et al.A novel Ni-Co alloy catalyst derived from spinel[J].Journal of Alloys and Compounds,2022,925:166600.
[23] Bautista F M,Campelo J M,Garcia A,et al.N-Alkylation of aniline with methanol over AlPO4Al2O3 catalysts[J].Applied Catalysis A:General,1998,166(1):39-45.
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