以反相微乳液法和沉淀法相结合制备了核壳结构TiO2@SiO2,首次用于碳酸二甲酯与苯酚酯交换合成碳酸二苯酯反应,显示较好的催化活性.采用200°C焙烧的TiO2@SiO2,用量0.20 g,反应9h,苯酚转化率达41.8%,酯交换选择性为100%.透射电镜显示TiO2@SiO2核厚壳薄, TiO2核直径220-300 nm, SiO2壳厚度40-60 nm,具有介孔结构. TiO2@SiO2对碳酸二甲酯与苯酚酯交换反应有好的重复使用性,使用4次苯酚转化率仍保持在40%以上. TiO2与SiO2发生相互作用, Ti进入骨架形成Ti-O-Si键,骨架Ti的形成提高了TiO2@SiO2的催化性能.
Core-shell TiO2@SiO2 was prepared using a combination of reverse microemulsion and precipita-tion methods and used as a heterogeneous catalyst for the transesterification of dimethyl carbonate and phenol. TiO2@SiO2 calcined at 200 °C gave the best catalytic performance. When the amount of catalyst was 0.20 g, the phenol conversion and transesterification selectivity were 41.8% and 100%, respectively. Transmission electron microscopy was used to characterize the core-shell TiO2@SiO2 structure, and the results showed that TiO2@SiO2 is bilayer with a TiO2 core of diameter 220-300 nm and SiO2 shell of thickness 40-60 nm. The TiO2@SiO2 was reusable, and phenol conversion re-mained above 40% when the TiO2@SiO2 was used four times. The catalytic performance of TiO2@SiO2 in the transesterification of dimethyl carbonate and phenol was promoted by the for-mation of Ti-O-Si bonds.
参考文献
[1] | Fukuoka S;Kawamura M;Komiya K;Tojo M Hachiya H Hasegawa K Aminaka M Okamoto H Fukawa I Konno S .[J].Green Chemistry,2003,5:497. |
[2] | 李碧静,葛鑫,陈彤,胡徐腾,王公应.苯酚酯交换合成碳酸二苯酯的多相催化剂研究进展[J].化工进展,2010(05):847-853. |
[3] | Kim Y T;Park E D .[J].Applied Catalysis A:General,2009,356:211. |
[4] | 罗淑文,陈彤,童东绅,曾毅,雷永诚,王公应.杂原子介孔分子筛Me-HMS催化酯交换合成碳酸二苯酯[J].催化学报,2007(11):937-939. |
[5] | Mei F M;Pei Z;Li G X .[J].Organic Process Research and Development,2004,8:372. |
[6] | Chen T;Han H J;Yao J;Wang G Y .[J].CATALYSIS COMMUNICATIONS,2007,8:1361. |
[7] | 陈彤;李碧静;胡晓佳;王公应 唐荣芝 杨建 刘旭冉 蔡家胜 .[P].CN Patent 103120934A,2013. |
[8] | Park OK;Kang YS .Preparation and characterization of silica-coated TiO2 nanoparticle[J].Colloids and Surfaces, A. Physicochemical and Engineering Aspects,2005(0):261-265. |
[9] | Hwang ST;Hahn YB;Nahm KS;Lee YS .Preparation and characterization of poly(MSMA-co-MMA)-TiO2/SiO2 nanocomposites using the colloidal TiO2/SiO2 particles via blending method[J].Colloids and Surfaces, A. Physicochemical and Engineering Aspects,2005(1/3):63-69. |
[10] | Wu L Z;Yu Y;Zhang Y;Li Y Z Zhang Y Zhi J F .[J].Journal of Colloid and Interface Science,2012,369:179. |
[11] | Wang S;Wang T;Chen WX;Hori TR .Phase-selectivity photocatalysis: a new approach in organic pollutants' photodecomposition by nanovoid core(TiO2)/shell(SiO2) nanoparticles[J].Chemical communications,2008(32):3756-3758. |
[12] | Ren, Y.;Chen, M.;Zhang, Y.;Wu, L. .Fabrication of rattle-type TiO_2/SiO_2 core/shell particles with both high photoactivity and UV-shielding property[J].Langmuir: The ACS Journal of Surfaces and Colloids,2010(13):11391-11396. |
[13] | 曹婷,孙立婷,石玉,华丽,张然,郭立,朱闻闻,侯震山.无机氧化物载体对催化 CO2 与环氧化合物合成环状碳酸酯的促进作用[J].催化学报,2012(03):416-424. |
[14] | 张海娇,刘月明,何鸣元,吴鹏.无机SiO2-TiO2前驱体体系合成高性能TS-1分子筛[J].催化学报,2006(09):749-751. |
[15] | 葛鑫,李碧静,胡静,陈彤,王公应,胡徐腾.焙烧温度对二氧化钛催化性能的影响[J].化学工程,2011(11):61-65. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%