丙烯环氧化制环氧丙烷是催化领域的最关键的挑战之一. 本文对作者等近年来开展的以一氧化二氮为氧化剂的铁催化体系和以氧气为氧化剂的铜催化体系的研究进展进行了综述. 在这两类催化体系中,碱金属离子(特别是K+)的修饰作用均是获得较高环氧丙烷选择性的关键. 碱金属离子通过调变催化剂中铁或铜物种的分散度、配位环境和酸碱性等,实现了对反应途径的调控,使反应朝着有利于环氧丙烷生成的方向进行. 活性金属组分(铁或铜)与氧化剂(一氧化二氮或氧气)间的特定的组合对丙烯环氧化反应的发生也起着重要作用. 推测在两类催化体系中,氧化剂均在具有特定结构和价态的铁或铜活性位上活化,产生导致丙烯环氧化反应发生的亲电性活性氧物种.
参考文献
[1] | Eissen M;Metzger J O;Schmidt E;Schneidewind U .[J].Angewandte Chemie International Edition,2002,41(03):414. |
[2] | Nijhuis TA;Makkee M;Moulijn JA;Weckhuysen BM .The production of propene oxide: Catalytic processes and recent developments[J].Industrial & Engineering Chemistry Research,2006(10):3447-3459. |
[3] | Clerici M G;Bellussi G;Romano U .[J].Journal of Catalysis,1991,129(01):159. |
[4] | Tullo A .[J].Chemical and Engineering News,2004,82(36):15. |
[5] | 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. |
[6] | Laufer W;Meiers R;Hlderich W .[J].Journal of Molecular Catalysis A:Chemical,1999,141(1-3):215. |
[7] | Laufer W;Hoelderich W F .[J].Applied Catalysis A:General,2001,213(02):163. |
[8] | Beckman E J .[J].Green Chemistry,2003,5(03):332. |
[9] | Kamata K.;Yonehara K.;Sumida Y.;Yamaguchi K.;Hikichi S.;Mizuno N. .Efficient epoxidation of olefins with >= 99% selectivity and use of hydrogen peroxide[J].Science,2003(5621):964-966. |
[10] | Xi Z W;Zhou N;Sun Y;Li K L .[J].Science,2001,292(5519):1139. |
[11] | Hayashi T.;Haruta M.;Tanaka K. .Selective vapor-phase epoxidation of propylene over Au/TiO2 catalysts in the presence of oxygen and hydrogen[J].Journal of Catalysis,1998(2):566-575. |
[12] | Uphade BS.;Tsubota S.;Haruta M.;Okumura M. .Effect of physical mixing of CsCl with Au/Ti-MCM-41 on the gas-phase epoxidation of propene using H-2 and O-2: Drastic depression of H-2 consumption[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2000(1/2):43-50. |
[13] | Uphade B S;Yamada Y;Akita T;Nakamura T Haruta M .[J].Applied Catalysis A:General,2001,215(1-2):137. |
[14] | Uphade B S;Akita T;Nakamura T;Haruta M .[J].Journal of Catalysis,2002,209(02):331. |
[15] | Sinha A K;Seelan S;Akita T;Tsubota S Haruta M .[J].Applied Catalysis A:General,2003,240(1-2):243. |
[16] | Qi C X;Okumura M;Akita T;Haruta M .[J].Applied Catalysis A:General,2004,263(01):19. |
[17] | Sinha A K;Seelan S;Tsubota S;Haruta M .[J].Angewandte Chemie International Edition,2004,43(12):1546. |
[18] | Sinha A K;Seelan S;Okumura M;Akita T Tsubota S Haruta M .[J].Journal of Physical Chemistry B,2005,109(09):3956. |
[19] | Daté M;Okumura M;Tsubota S;Haruta M .[J].Angewandte Chemie International Edition,2004,43(16):2129. |
[20] | Chowdhury B;Bravo-Suárez J J;Daté M;Tsubota S Haruta M .[J].Angewandte Chemie International Edition,2006,45(03):412. |
[21] | Panov G I .[J].Cattech,2000,4(01):18. |
[22] | Pérez-Ramírez J;Kondratenko E V.[J].Chemical Communications,2003(17):2152. |
[23] | Wang X X;Wang Y;Tang Q H;Guo Q Zhang Q H Wan H L .[J].Journal of Catalysis,2003,217(02):457. |
[24] | Dubkov K A;Ovanesyan N S;Shteinman A A;Starokon E V Panov G I .[J].Journal of Catalysis,2002,207(02):341. |
[25] | Jia J F;Pillai K S;Sachtler W M H .[J].Journal of Catalysis,2004,221(01):119. |
[26] | Panov G I;Starokon E V;Pirutko L V;Paukshtis E A Parmon V N .[J].Journal of Catalysis,2008,254(01):110. |
[27] | Xia H A;Sun K Q;Sun K J;Feng Z C Li W X Li C .[J].Journal of Physical Chemistry C,2008,112(24):9001. |
[28] | Duma V.;Honicke D. .Gas phase epoxidation of propene by nitrous oxide over silica-supported iron oxide catalysts[J].Journal of Catalysis,2000(1):93-104. |
[29] | Wang X X;Zhang Q H;Guo Q;Lou Y Ch Yang L J Wang Y.[J].Chemical Communications,2004(12):1396. |
[30] | Wang X X;Zhang Q H;Yang S F;Wang Y .[J].Journal of Physical Chemistry B,2005,109(49):23500. |
[31] | Wang Y;Yang W;Yang L J;Wang X X Zhang Q H .[J].Catalysis Today,2006,117(1-3):156. |
[32] | Zhang Q H;Guo Q;Wang X X;Shishido T Wang Y .[J].Journal of Catalysis,2006,239(01):105. |
[33] | 郭倩,汪晓星,张庆红,王野.K+-FeOx/SBA-15催化剂中共存阴离子对其丙烯环氧化性能的影响[J].厦门大学学报(自然科学版),2005(05):593-595. |
[34] | Yang S F;Zhang Q H;Wang Y .[J].Chemistry Letters,2007,36(06):786. |
[35] | Yang S F;Zhu W M;Zhang Q H;Wang Y .[J].Journal of Catalysis,2008,254(02):251. |
[36] | Ananieva E;Reitzmann A .Direct gas-phase epoxidation of propene with nitrous oxide over modified silica supported FeOx catalysts[J].Chemical Engineering Science,2004(22/23):5509-5517. |
[37] | Costine A;O'Sullivan T;Hodnett B K .[J].Catalysis Today,2006,112(1-4):103. |
[38] | Moens B;De Winne H;Corthals S;Poelman H De Gryse R Meynen V Cool P Sels B F Jacobs P A .[J].Journal of Catalysis,2007,247(01):86. |
[39] | Ross J .[J].Applied Catalysis,1991,69(02):N19. |
[40] | McCoy M .[J].Chemical and Engineering News,2001,79(43):12. |
[41] | Monnier J R .[J].Applied Catalysis A:General,2001,221(1-2):73. |
[42] | Pitchai R;Kahn A P;Gaffney A M .[P].US 5625084,1997. |
[43] | Cooker B;Gaffney A M;Jewson J D;Onimus W H .[P].US 5780657,1998. |
[44] | Lu GZ.;Zuo XB. .Epoxidation of propylene by air over modified silver catalyst[J].Catalysis Letters,1999(1):67-70. |
[45] | Zemichael F W;Palermo A;Tikhov M S;Lambert R M .[J].Catalysis Letters,2002,80(3-4):93. |
[46] | 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. |
[47] | Takahashi A;Hamakawa N;Nakamura I;Fujitani T .[J].Applied Catalysis A:General,2005,294(01):34. |
[48] | Lu JQ;Bravo-Suarez JJ;Takahashi A;Haruta M;Oyama ST .In situ UV-vis studies of the effect of particle size on the epoxidation of ethylene and propylene on supported silver catalysts with molecular oxygen[J].Journal of Catalysis,2005(1):85-95. |
[49] | Lu JQ;Bravo-Suarez JJ;Haruta M;Oyama ST .Direct propylene epoxidation over modified Ag/CaCO3 catalysts[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(2):283-295. |
[50] | Lambert RM;Williams FJ;Cropley RL;Palermo A .Heterogeneous alkene epoxidation: past, present and future[J].Journal of molecular catalysis, A. Chemical,2005(1/2):27-33. |
[51] | Cropley R L;Williams F J;Vaughan O P H;Urquhart A J Tikhov M S Lambert R M .[J].Surface Science,2005,578(1-3):L85. |
[52] | Cropley, RL;Williams, FJ;Urquhart, AJ;Vaughan, OPH;Tikhov, MS;Lambert, RM .Efficient epoxidation of a terminal alkene containing allylic hydrogen atoms: trans-methylstyrene on Cu{111}[J].Journal of the American Chemical Society,2005(16):6069-6076. |
[53] | Monnier J R;Hartley G W .[J].Journal of Catalysis,2001,203(01):253. |
[54] | 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. |
[55] | 鲁继青,罗孟飞,李灿.Cu/SiO2催化剂上丙烯在空气中的直接环氧化反应[J].催化学报,2004(01):5-9. |
[56] | Vaughan O P H;Kyriakou G;Macleod N;Tikhov M Lambert R M .[J].Journal of Catalysis,2005,236(02):401. |
[57] | Chu H;Yang L J;Zhang Q H;Wang Y .[J].Journal of Catalysis,2006,241(01):225. |
[58] | Wang Y;Chu H;Zhu W M;Zhang Q H .[J].Catalysis Today,2008,131(1-4):496. |
[59] | Zhu W M;Zhang Q H;Wang Y .[J].Journal of Physical Chemistry C,2008,112(20):7731. |
[60] | Inui T;Ueda T;Suehiro M .[J].Journal of Catalysis,1980,65(01):166. |
[61] | Reitz JB.;Solomon EI. .Propylene oxidation on copper oxide surfaces: Electronic and geometric contributions to reactivity and selectivity[J].Journal of the American Chemical Society,1998(44):11467-11478. |
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