小粒径Fe_3O_4磁粉的制备及其在有机合成中的应用
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摘要
采用简易化共沉淀氧化法,以盐酸酸洗碳钢废液为原料制备Fe_3O_4磁粉。通过反应过程中pH的变化监测反应溶液中的n(Fe~(3+))∶n(Fe~(2+)),为氧化共沉淀法提供了简易化操作。比较了制备的小粒径(18～20nm)Fe_3O_4与Alfa试剂级50～100 nm粒径的Fe_3O_4在香豆素衍生物和喹喔啉衍生物合成中的催化效果。结果表明,自制Fe_3O_4的催化效果较好、产率较高,且明显缩短了反应时间。采用振动样品磁强计、X射线衍射仪、TEM对制备的Fe_3O_4样品进行了表征;化合物的结构均经核磁共振波谱(NMR)和高分辨质谱(HRMS)确证。
The Fe_3O_4 magnetic powder was prepared with simple co-precipitation oxidation method using steel pickling waste liquor as raw material. The mole ratio of Fe3+∶Fe~(2+) in the reaction solution was monitored by the change of pH during the reaction process, which provided a simple operation for the co-precipitation oxidation method. The catalytic effect of Fe_3O_4 with small particle size of 18～20 nm and Alfa reagent grade of 50～ 100 nm on the synthesis of coumarin derivatives and quinoxaline derivatives was compared. The self-made Fe_3O_4 has a good catalytic reaction effect, high yield, and significantly shortens the reaction time. The prepared Fe_3O_4 samples were characterized by VSM, XRD and TEM. The structures of the compounds were confirmed by nuclear magnetic resonance spectroscopy(NMR) and high resolution mass spectrometry(HRMS).
The Fe_3O_4 magnetic powder was prepared with simple co-precipitation oxidation method using steel pickling waste liquor as raw material. The mole ratio of Fe3+∶Fe~(2+) in the reaction solution was monitored by the change of pH during the reaction process, which provided a simple operation for the co-precipitation oxidation method. The catalytic effect of Fe_3O_4 with small particle size of 18～20 nm and Alfa reagent grade of 50～ 100 nm on the synthesis of coumarin derivatives and quinoxaline derivatives was compared. The self-made Fe_3O_4 has a good catalytic reaction effect, high yield, and significantly shortens the reaction time. The prepared Fe_3O_4 samples were characterized by VSM, XRD and TEM. The structures of the compounds were confirmed by nuclear magnetic resonance spectroscopy(NMR) and high resolution mass spectrometry(HRMS).
引文
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[20]Aamer S,Aliya I.Synthesis of Some new 3-(5-(arylamino)-1,3,4-thiadiazol-2-yl)-2H-chromen-2-ones and 3-(4-aryl-5-thioxo-4,5-dihydro-1H-1,2,4-triazol-3-YL)-2H-chromen-2-ones[J].Phosphorus Sulfur and Silicon,2011,186:1801-1810.
[2]Sun Anni(孙安妮),Sun Genhang(孙根行).Research progress in regeneration and utilization of waste hydrochloric acid[J].Contemporary Chemical Industry(当代化工),2011,40(11):1178-1181.
[3]Wan Guangqin(万光琴).The preparation of iron oxide red from iron and steel pickling waste liquor and its industrialization[D].Tianjin:Tianjin University(天津大学),2017.
[4]Liu S J,Yang H Y,Yang Y K,et al.Novel co-precipitation-oxidation method for recovering iron from steel waste pickling liquor[J].Frontiers of Environmental Science&Engineering,2017,11(1):89-98..
[5]Wang Xingyao(王兴尧),Lv Feifei(吕飞飞).Synthesis of Fe3O4Magnetic powder from spent pickling liquors[J].Trans Tianjin Univ(天津大学学报),2018,24:45-50.
[6]He K,Xu C Y,Zhen L,et al.Hydrothermal synthesis and characterization of single-crystalline Fe3O4,nanowires with high aspect ratio and uniformity[J].Materials Letters,2007,61(14/15):3159-3162.
[7]Hong R Y,Pan T T,Li H Z.Microwave synthesis of magnetic Fe3O4,nanoparticles used as a precursor of nanocomposites and ferrofluids[J].Journal of Magnetism&Magnetic Materials,2006,303(1):60-68.
[8]Zou Tao(邹涛),Guo Canxiong(郭灿雄),Duan Xue(段雪),et al.Preparation and characterization of nano-size Fe3O4 particles with strong magnetism[J].Fine Chemicals(精细化工),2002,19(12):707-710.
[9]Ma Cong(马聪).Study on preparation of Fe3O4 magnetic powder for developer by waste steel pickling[D].Tianjin:Tianjin University(天津大学),2013.
[10]Lv Feifei(吕飞飞).The investigation of is synthesis of Fe3O4magnetic powder from spent pickling liquors[D].Tianjin:Tianjin University(天津大学),2017.
[11]Hong Y L,Shu H Y,Jia D,et al.Magnetic Fe3O4 nanoparticles as new,efficient,and reusable catalysts for the synthesis of quinoxalines in water[J].Aust J Chem,2010,63:1290-1296.
[12]Mojtahedi M M,Abaee M S,Alishiri T.Superparamagnetic iron oxide as an efficient catalyst for the one-pot,solvent-free synthesis ofα-aminonitriles[J].Tetrahedron Letters,2009,50(20):2322-2325.
[13]Chen Yajie(陈亚杰),Lin Shangxin(林赏心),Pu Jixiong(蒲继雄).Preparation and catalytic performance of Fe3O4 nanoparticles[J].Joural of Huaqiao University(华侨大学学报),2015,36(5):541-545.
[14]Soumen P,Arijit S,Subhash B.Magnetically recoverable Fe3O4nanoparticles for the one-pot synthesis of coumarin-3-carboxamide derivatives in aqueous ethanol[J].Chemistry Select Communications,2018,3:7535-7540.
[15]Misawa T,Hashimoto K,Shimodaira S.The mechanism of formation of iron oxide and oxyhydroxides in aqueous solutions at room temperature[J].Corrosion Science,1974,5(16).DOI:10.1002/chin.197416032.
[16]Yang Xiyun(杨喜云),Gong Zhuqing(龚竹青),Peng Changhong(彭长宏),et al.Formation mechanism of magnetite prepared by air oxidation[J].Journal of Central south University(中南大学学报),2008,39(3):454-458.
[17]Zhang Yonggang(张永刚),Gao Yanan(高亚男).Fe3+and Fe2+determination in steel pickling waste acid liquor[J].Journal of Tianjin Polytechnic University(天津工业大学学报),2008,27(4):39-40.
[18]Bull A A.Synthesis and antimicrobial activity of some nitrogen heterocycles incorporation into coumarin[J].Nahed Fadel Abdel Ghaffar,2009,20(1):51-59.
[19]Daniela S,Simone C,Adriana B,et al.Synthesis and selective human monoamine oxidase inhibition of 3-carbonyl,3-acyl,and3-carboxyhydrazido coumarin derivatives[J].European Journal of Medicinal Chemistry,2011,46(10):4846-4852.
[20]Aamer S,Aliya I.Synthesis of Some new 3-(5-(arylamino)-1,3,4-thiadiazol-2-yl)-2H-chromen-2-ones and 3-(4-aryl-5-thioxo-4,5-dihydro-1H-1,2,4-triazol-3-YL)-2H-chromen-2-ones[J].Phosphorus Sulfur and Silicon,2011,186:1801-1810.
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