以钛酸正丁酯为原料采用原位化学合成的新方法,以二价钴离子为模板剂在TiO2凝胶基质合成的同时,通过邻苯二腈的四聚反应将酞菁钴(CoPc)在TiO2表面原位合成,得到均匀掺杂的CoPc/TiO2光催化剂.用紫外-可见漫反射光谱、傅立叶变换-红外光谱等证实了CoPc的成功负载,并将其用于可见光下、水溶液中CO2的还原反应,通过比较还原反应的效率,确定此光催化剂的最佳制备条件为:CoPc在TiO2表面的摩尔负载量为3%,焙烧温度为200℃,溶胶搅拌时间为20 h,钛酸丁酯与邻苯二腈及钴离子同时加入溶胶体系中.采用此法制备的催化剂中CoPc酞菁环上的电子密度增加,有利于作为敏化剂的激发态CoPc向半导体TiO2的导带注入电子,而且CoPc被均匀分散于TiO2凝胶基质中,其上的"笼效应"有效避免了CoPc的迁移,使其二聚及多聚倾向大大减弱.此光催化剂用于CO2光还原,在可见光照射下,水溶液中即可光还原CO2为甲醇、甲醛、甲酸等产物,在光照反应10 h后总产量最高可达2903.83 μmol/ g-catal.
参考文献
| [1] | Takaynki M;Kengi A;Ohta K et al.Effect of CO2 pressure on photocatalytie reduction of CO2 using TiO2 in aqueous solutions[J].Journal of Photochemistry and Photobiology A:Chemistry,1996,9s(1-2):87-90. |
| [2] | G. R. Dey;A. D. Belapurkar;K. Kishore .Photo-catalytic reduction of carbon dioxide to methane using TiO_2 as suspension in water[J].Journal of Photochemistry and Photobiology, A. Chemistry,2004(3):503-508. |
| [3] | Lobsnov A V;Kholuiskaya S N;Komissarov G G .Photocatalytie synthesis of formaldehyde from CO2 and H2O2[J].Daklady Phys Chem,2004,399(1-3):266-268. |
| [4] | Keita Ikeue;Shinjiro Nozaki;Makoto Ogawa;Masakazu Anpo .Photocatalytic reduction of CO_2 with H_2O on Ti-containing porous silica thin film photocatalysts[J].Catalysis Letters,2002(3/4):111-114. |
| [5] | Nguyen TV;Wu JCS .Photoreduction of CO2 to fuels under sunlight using optical-fiber reactor[J].Solar Energy Materials and Solar Cells: An International Journal Devoted to Photovoltaic, Photothermal, and Photochemical Solar Energy Conversion,2008(8):864-872. |
| [6] | I-Hsiang T;Jeffrey CS W .Chemical states of metal-loaded titania in the photoreduetion of CO2[J].Catalysis Today,2004,97(2-3):113-119. |
| [7] | Premkumar J;Ramaraj R .Phowcatalytie reduction of carbon dioxide to formic acid at porphyrin and phttmloeyanine adsorbed Nation membranes[J].Journal of Photochemistry and Photobiology A:Chemistry,1997,110(01):53-58. |
| [8] | I-Hsiang Tseng;Wan-Chen Chang;Jeffrey C.S.Wu .Photoreduction of CO_2 using sol-gel derived titania and titania-supported copper catalysts[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2002(1):37-48. |
| [9] | G. A. KUMAR;J. THOMAS;N. GEORGE .Physical and optical properties of phthalocyanine doped inorganic glasses[J].Journal of Materials Science,2000(10):2539-2542. |
| [10] | 赵志换;范济民;王志忠 .变色酸分光光度法测定苛性溶液中的甲酸钠[J].分析试验室,2005,24(Sup):272-275. |
| [11] | Uchlda H;Sosaki T;Ogura K .Dark catalytic reduction of CO2 over prussian blue-deposited TiO2 and the photo reactivation of the catalyst[J].Journal of Molecular Catalysis,1994,93(03):269-277. |
| [12] | 黄金陵,彭亦如,陈耐生.金属酞菁配合物结构研究的一些谱学方法[J].光谱学与光谱分析,2001(01):1-6. |
| [13] | Zhan H B;Wang M Q;Chen W Z .In situ synthesis of metallo-phthaloeyanines in inorganic matrix[J].Materials Letters,2000,55:97-103. |
| [14] | Zhan H B;Chen W Z;Li G H et al.Dimerization of metallopholocyanines in inorganic matrix[J].Materials Science and Engineering B:Solid State Materials for Advanced Technology,2003,100:113-118. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%