在423 K、常压固定床石英反应器中,以丙烯直接气相氧化为探针反应,考察了催化剂制备方法、沉淀剂的种类和浓度对制备的Ag/TS-1催化剂催化性能的影响,采用TEM,XRD和UV-Vis等表征手段对Ag/TS-1催化剂进行了分析. 结果表明,沉积-沉淀法是最佳的催化剂制备方法,但浸渍法也可制得具有环氧丙烷选择性的催化剂. K2CO3是一种良好的沉淀剂. 以K2CO3为沉淀剂,硅钛比为64的TS-1为载体制备的Ag/TS-1催化剂上的丙烯转化率为1.72%,环氧丙烷选择性为98.2%. 少量单质银的存在有利于环氧丙烷的生成,除银粒子的分散状态外,银粒子与载体TS-1间的相互作用对提高催化剂的选择性具有决定性作用.
参考文献
[1] | Ainsworth S J .[J].Chemical and Engineering News,1992,70(24):9. |
[2] | Taramasso M;Perego G;Notari B .[P].US 4 410 501,1983. |
[3] | Taramasso M;Manara G;Fattore V .[P].US 4 666 692,1987. |
[4] | Uphade BS.;Hayashi T.;Haruta M.;Tsubota S. .Selective oxidation of propylene to propylene oxide or propionaldehyde over Au supported on titanosilicates in the presence of H-2 and O-2[J].Chemistry Letters,1998(12):1277-1278. |
[5] | Uphade B S;Akita T;Nakamura T;Haruta M .[J].Journal of Catalysis,2002,209(02):331. |
[6] | Uphade B S;Yamade Y;Akita T .[J].Applied Catalysis A:General,2001,215:137. |
[7] | Uphade B S;Okumura M;Yamade N;Tsubota S,Haruta M .[J].Studies in Surface Science and Catalysis,2000,130A:833. |
[8] | Xi Z W;Zhou N;Sun Y;Li K L .[J].Science,2001,292(5519):1139. |
[9] | Meiers R.;Holderich WF.;Dingerdissen U. .Synthesis of propylene oxide from propylene, oxygen, and hydrogen catalyzed by palladium-platinum-containing titanium silicalite[J].Journal of Catalysis,1998(2):376-386. |
[10] | Jenzer G;Mallat T;Maciejewski M .[J].Applied Catalysis A:General,2001,208:125. |
[11] | Lu G Zh;Zuo X B .[J].Catalysis Letters,1999,58(01):67. |
[12] | Lu JQ.;Luo MF.;Lei H.;Li C. .Epoxidation of propylene on NaCl-modified silver catalysts with air as the oxidant[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2002(1/2):11-19. |
[13] | Zemichael F W;Palermo A;Tikhov M S;Lambert R M .[J].Catalysis Letters,2002,80(3-4):93. |
[14] | Lu JQ.;Luo MF.;Lei H.;Bao XH.;Li C. .Epoxidation of propylene on NaCl-modified VCe1-xCux oxide catalysts with direct molecular oxygen as the oxidant[J].Journal of Catalysis,2002(2):552-555. |
[15] | 金国杰,卢冠忠,王新宏.丙烯气相一步氧化制环氧丙烷用Ag-Mo催化剂的研究[J].催化学报,2002(05):405-407. |
[16] | Oliveira A L;Wolf A;Schüth F .[J].Catalysis Letters,2001(73):157. |
[17] | Haruta M;Uphade B S;Tsubota S;Miyamoto A .[J].Research on Chemical Intermediates,1998,24(03):329. |
[18] | 王瑞璞,郭新闻,王祥生.直接催化氧化法合成环氧丙烷研究进展[J].化工学报,2003(01):2-8. |
[19] | Li G;Guo X W;Wang X Sh .[J].Applied Catalysis A:General,1999,185:11. |
[20] | Tsubota S;Cunningham D A H;Bando Y;Haruta M .[J].Studies in Surface Science and Catalysis,1995,91:227. |
[21] | 王瑞璞,郝敬泉,郭新闻,王祥生.氢氧混合体系下Ag/TS-1催化剂上丙烯的高效环氧化反应[J].催化学报,2003(05):319-320. |
[22] | 王瑞璞;郝敬泉;郭新闻;王祥生.[J].石油学报(石油加工) |
[23] | Vayssilov GN .Structural and physicochemical features of titanium silicalites[J].Catalysis Reviews. Science and Engineering,1997(3):209-251. |
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