Ag_N_TiO_2_SBA_1_省略_的制备及其可见光催化还原CO_2_高梦语.docxVIP

化 学 学 报Article研究论文ACTA CHIMICA SINICADOI: 10.6023/g/N-TiO2/SBA-15 光催化剂的制备及其可见光催化还原 CO2高梦语a,b姜东*,a孙德魁a侯博 a李德宝a(a中国科学院山西煤炭化学研究所 煤转化国家重点实验室 太原 030001)(b中国科学院大学 北京 100049)摘要 以钛酸四正丁酯(TB), 羧基改性的 SBA-15(COOH/SBA-15), 尿素和 AgNO3为原料, 利用溶剂热及焙烧处理制Ag/N-TiO2/SBA-15 催化剂. 采用X 射线衍射(XRD), 低温N2吸脱附, X 射线光电子能谱(XPS), 紫外-可见漫反射光(UV-vis DRS), 荧光(PL) 光谱, 电感耦合等离子体原子发射光谱(ICP) 和元素分析(EA) 等表征. 结果显示:Ag/N-TiO2/SBA-15 样品具有介孔结构, TiO2以单一的锐钛矿晶型均匀的分散在载体表面, Ag 以单质形态沉积在 TiO2表面, N 则掺入到 TiO2 晶格中, 并以取代 N(O-Ti-N)和间隙 N(Ti-O-N)两种方式共存. Ag/N-TiO2/SBA-15 催化剂中单质Ag 既可以捕获光生电子提高量子效率, 又促进了 TiO2对可见光的吸收. N 掺杂拓宽了 TiO2吸收光谱的吸收范围, 并且适量的 N 掺杂有助于光生电荷的分离, 提高了光催化效率. 以光催化还原 CO2 为探针反应, 考察了催化剂在可见光下 的催化活性. 结果表明: Ag/N-TiO2/SBA-15 系列催化剂均表现出了可见光催化还原CO2 性能, 发现当Ag 的质量分数为 2%, N 与 Ti 的物质的量比为 3 时, 催化剂光催化活性最佳, 产物甲醇产量高达 45.7 μmol?g－1?h－1.关键词 TiO2; 羧基改性 SBA-15; Ag 沉积; N 掺杂; 可见光; 光催化还原 CO2Synthesis of Ag/N-TiO2/SBA-15 Photocatalysts and Photocatalytic Reduction of CO2 under Visible Light IrradiationGao, Mengyua,bJiang, Dong*,aSun, DekuiaHou, BoaLi, Debaoa(aState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001)(bUniversity of Chinese Academy of Sciences, Beijing 100049)Abstract Silver-loaded together with nitrogen-doped highly dispersed TiO2/SBA-15 mesoporous catalysts were success-fully synthesized through solvothermal treatment and calcination method by using titanium n-butoxide (TB), carbox-ylate-modified SBA-15 (COOH/SBA-15), urea and silver nitrate as raw materials. The detailed preparation procedure was as follows: 1.0 g COOH/SBA-15 powder was dispersed in solution containing 0.82 mL titanium n-butoxide (TB) and 20.0 mL acetic ether. The mixture was stirred for 30 min at room temperature, then 0.031 g AgNO3 was added into the solution by further stirring for 30 min and a certain amount of urea was added. After being stirred continuously for 3 h, the resultant solu-tion was transferred into a teflon-lined stainless autoclave and solvothermally treated at 220 ℃ for 12 h. A