磁性硅基固体酸的制备及性能研究
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摘要
以水热法制备的Fe_3O_4为磁核,采用溶胶凝胶法合成磁性SiO_2,最后通过浸渍法制备磁性硅基固体酸,以乙酸和乙醇的酯化反应为探针考察其催化活性。使用扫描电子显微镜、透射电子显微镜、X射线衍射分析、傅里叶转换红外光谱、振动样品磁强计对Fe_3O_4、磁性SiO_2和固体酸进行表征,并研究了不同反应条件对磁性SiO_2的磁性性能和固体酸催化性能的影响,实验结果表明:制备的Fe_3O_4具有超顺磁性,其饱和磁化强度高达67. 02 A·m~2/kg,磁性SiO_2和磁性硅基固体酸也均具有较强的磁性。在n(TEOS)∶n(氨水)∶n(乙醇)=1∶4∶20时,固体酸的酯化率达到69. 68%,酸量达到2. 345 mmol/g。
Fe_3O_4 was prepared by hydrothermal method,and was used as magnetic core to synthesize magnetic SiO_2 by sol-gel method. The magnetic silica-based solid acid catalyst was prepared by impregnation method and the catalytic activity was investigated by esterification reaction of acetic acid and ethanol. Fe_3O_4,magnetic SiO_2 and the magnetic silica-based solid acid catalyst were characterized by means of scanning electron microscope,transmission electron microscope,X-ray diffraction,Fourier transform infrared spectroscopy and vibrating sample magnetometer.The effects of different reaction conditions on the magnetic property of magnetic SiO_2 and the catalytic property of solid acid were discussed. The results show that the prepared Fe_3O_4 exhibits super paramagnetic property and high saturation magnetization of 67. 02 A · m~2/kg. Magnetic SiO_2 and magnetic silica-based solid acid catalyst also exhibit strong magnetic property. At n( TEOS) ∶ n( ammonia) ∶ n( ethanol) = 1 ∶ 4 ∶ 20,the esterification rate of solid acid catalyst runs up to 69. 68 %,and the acid amount reaches 2. 345 mmol/g.
Fe_3O_4 was prepared by hydrothermal method,and was used as magnetic core to synthesize magnetic SiO_2 by sol-gel method. The magnetic silica-based solid acid catalyst was prepared by impregnation method and the catalytic activity was investigated by esterification reaction of acetic acid and ethanol. Fe_3O_4,magnetic SiO_2 and the magnetic silica-based solid acid catalyst were characterized by means of scanning electron microscope,transmission electron microscope,X-ray diffraction,Fourier transform infrared spectroscopy and vibrating sample magnetometer.The effects of different reaction conditions on the magnetic property of magnetic SiO_2 and the catalytic property of solid acid were discussed. The results show that the prepared Fe_3O_4 exhibits super paramagnetic property and high saturation magnetization of 67. 02 A · m~2/kg. Magnetic SiO_2 and magnetic silica-based solid acid catalyst also exhibit strong magnetic property. At n( TEOS) ∶ n( ammonia) ∶ n( ethanol) = 1 ∶ 4 ∶ 20,the esterification rate of solid acid catalyst runs up to 69. 68 %,and the acid amount reaches 2. 345 mmol/g.
引文
[1]支德福,白宇超,张琳,等.基于超顺磁Fe3O4的磁响应型纳米药物载体的研究进展[J].化学通报,2017,80(11):987-994.
[2]李莉,莫尊理,郭瑞斌,等.表面修饰磁性Fe3O4粒子及其在生物医学应用中的新进展[J].功能材料,2016,47(4):28-32.
[3]刘天辉,常刚,曹瑞军,等.超顺磁性Fe3O4纳米粒子在磁共振造影中的应用[J].化学进展,2015,27(5):601-613.
[4]赵涛.微波多元醇法合成Fe3O4纳米颗粒及其用于血管磁共振增强成像的应用基础研究[D].上海:上海交通大学,2014.
[5]肖旺钏,纪孝峰,郑英,等.超顺磁Fe3O4纳米粒子的制备及弛豫性能[J].人工晶体学报,2017(12):2478-2484.
[6]孙晓宁.碘化油磁流体纳米颗粒的制备及其在肿瘤热疗中的应用[D].济南:山东大学,2016.
[7]WANG D,DUAN X,ZHANG J,et al.Fabrication of superparamagnetic hydroxyapatite with highly ordered three-dimensional pores[J].Journal of Materials Science,2009,44(15):4020-4025.
[8]黄水仙,许熠铭,谢民强.磁性纳米颗粒在肿瘤治疗中的应用[J].中国中西医结合耳鼻咽喉科杂志,2013(3):237-240.
[9]陈林,霍红娜,孙立丽,等.Fe3O4磁性纳米粒子对花旗松素的吸附性能研究[J].天津中医药大学学报,2017,36(1):49-53.
[10]MAKENA P S,PIERCE S C,CHUNG K T,et al.Comparative mutagenic effects of structurally similar flavonoids quercetin and taxifolin on tester strains Salmonella typhimurium TA102 and Escherichia coli WP-2 uvr A[J].Environmental&Molecular Mutagenesis,2010,50(6):451-459.
[11]黎人恺.Fe3O4磁性纳米粒子在中药成分分离分析中的应用研究[D].长沙:湖南师范大学,2015.
[12]涂丽君,宋平新,宋小会,等.超顺磁性Fe3O4@Si O2复合纳米粒子的制备、表征和性能研究[J].人工晶体学报,2015,44(4):1025-1030.
[13]王书宪.超顺磁性Fe3O4纳米粒子的Si O2包覆及磁共振性能研究[D].青岛:青岛科技大学,2014.
[14]郑杨,姜诚,韩德艳.磁性介孔二氧化硅微球的研究及应用进展[J].化学与生物工程,2014,31(2):19-22.
[15]刘冰,王德平,黄文旵,等.溶胶-凝胶法制备核壳Si O2/Fe3O4复合纳米粒子的研究[J].无机材料学报,2008,23(1):33-38.
[16]许谦.磁性纳米二氧化硅表面修饰及其应用[D].武汉:武汉工程大学,2015.
[17]王显祥,王森,杨婉身,等.超声合成Fe3O4@Si O2复合纳米磁性粒子用于质粒DNA的提纯[J].化学学报,2009,67(1):54-58.
[18]胡小兵.Fe3O4@Si O2核壳结构磁性纳米颗粒的制备研究[J].应用化工,2016,45(2):387-388.
[19]LI J,LIANG X.Magnetic solid acid catalyst for biodiesel synthesis from waste oil[J].Energy Conversion&Management,2017,141:126-132.
[20]许文艳.超顺磁性Fe3O4亚微米空心微球的制备及性能研究[D].武汉:武汉理工大学,2014.
[2]李莉,莫尊理,郭瑞斌,等.表面修饰磁性Fe3O4粒子及其在生物医学应用中的新进展[J].功能材料,2016,47(4):28-32.
[3]刘天辉,常刚,曹瑞军,等.超顺磁性Fe3O4纳米粒子在磁共振造影中的应用[J].化学进展,2015,27(5):601-613.
[4]赵涛.微波多元醇法合成Fe3O4纳米颗粒及其用于血管磁共振增强成像的应用基础研究[D].上海:上海交通大学,2014.
[5]肖旺钏,纪孝峰,郑英,等.超顺磁Fe3O4纳米粒子的制备及弛豫性能[J].人工晶体学报,2017(12):2478-2484.
[6]孙晓宁.碘化油磁流体纳米颗粒的制备及其在肿瘤热疗中的应用[D].济南:山东大学,2016.
[7]WANG D,DUAN X,ZHANG J,et al.Fabrication of superparamagnetic hydroxyapatite with highly ordered three-dimensional pores[J].Journal of Materials Science,2009,44(15):4020-4025.
[8]黄水仙,许熠铭,谢民强.磁性纳米颗粒在肿瘤治疗中的应用[J].中国中西医结合耳鼻咽喉科杂志,2013(3):237-240.
[9]陈林,霍红娜,孙立丽,等.Fe3O4磁性纳米粒子对花旗松素的吸附性能研究[J].天津中医药大学学报,2017,36(1):49-53.
[10]MAKENA P S,PIERCE S C,CHUNG K T,et al.Comparative mutagenic effects of structurally similar flavonoids quercetin and taxifolin on tester strains Salmonella typhimurium TA102 and Escherichia coli WP-2 uvr A[J].Environmental&Molecular Mutagenesis,2010,50(6):451-459.
[11]黎人恺.Fe3O4磁性纳米粒子在中药成分分离分析中的应用研究[D].长沙:湖南师范大学,2015.
[12]涂丽君,宋平新,宋小会,等.超顺磁性Fe3O4@Si O2复合纳米粒子的制备、表征和性能研究[J].人工晶体学报,2015,44(4):1025-1030.
[13]王书宪.超顺磁性Fe3O4纳米粒子的Si O2包覆及磁共振性能研究[D].青岛:青岛科技大学,2014.
[14]郑杨,姜诚,韩德艳.磁性介孔二氧化硅微球的研究及应用进展[J].化学与生物工程,2014,31(2):19-22.
[15]刘冰,王德平,黄文旵,等.溶胶-凝胶法制备核壳Si O2/Fe3O4复合纳米粒子的研究[J].无机材料学报,2008,23(1):33-38.
[16]许谦.磁性纳米二氧化硅表面修饰及其应用[D].武汉:武汉工程大学,2015.
[17]王显祥,王森,杨婉身,等.超声合成Fe3O4@Si O2复合纳米磁性粒子用于质粒DNA的提纯[J].化学学报,2009,67(1):54-58.
[18]胡小兵.Fe3O4@Si O2核壳结构磁性纳米颗粒的制备研究[J].应用化工,2016,45(2):387-388.
[19]LI J,LIANG X.Magnetic solid acid catalyst for biodiesel synthesis from waste oil[J].Energy Conversion&Management,2017,141:126-132.
[20]许文艳.超顺磁性Fe3O4亚微米空心微球的制备及性能研究[D].武汉:武汉理工大学,2014.