以碱性阴离子交换树脂Amberlite IRA-900为载体, Pd(C3H5)(C5H5)为金属有机前体,采用金属有机气相沉积法在室温下制备了Pd@IRA-900多相催化材料.紫外-可见光谱分析证明前体和树脂骨架之间的化学作用以及树脂本身的孔道结构使得Pd纳米粒子均匀分散在载体上.透射电镜结果显示钯纳米粒子的平均尺寸为2.6 nm.在较温和的条件下Pd@IRA-900对多种卤代芳烃和苯硼酸的Suzuki偶联都具有良好的催化活性,并且催化剂重复使用5次之后依然具有很好的活性.此外,对树脂载体进行碱性交换处理后可得到一种双功能催化材料Pd@IRA-900(OH),该催化剂在不加入碱的条件下也可以催化碘苯和苯硼酸的Suzuki偶联反应.
A basic anion exchange resin, Amberlite IRA-900, was loaded with Pd(C3H5)(C5H5) by an easy met-al-organic chemical vapor deposition (MOCVD) approach to give Pd@IRA-900 catalyst after reduc-tion at room temperature. Ultraviolet-Visible spectroscopy results showed a red shift of the absorp-tion peak of Pd2+after the Pd precursor was loaded on the resin, indicating that a chemical reaction occurred between the precursor and the support. Pd nanoparticles with 2.6 nm of average size were well dispersed on the support. The Pd@IRA-900 catalyst showed high activity for different kinds of aryl halides in Suzuki-Miyaura coupling reactions under mild and aerobic conditions. Excellent recyclability of Pd@IRA-900 catalyst was also observed in the Suzuki-Miyaura coupling reaction of iodobenzene and phenylboronic acid. A bifunctional catalyst Pd@IRA-900(OH) was synthesized by pretreating the ion exchange resin support with NaOH before Pd loading, which successfully cata-lyzed the Suzuki-Miyaura reaction of iodobenzene and phenylboronic acid without base under aer-obic conditions.
参考文献
[1] | Yin L;Liebscher J .[J].CHEMICAL REVIEWS,2007,107:133. |
[2] | Garrett C E;Prasad K .[J].Advanced Synthesis and Catalysis,2004,346:889. |
[3] | Welch CJ;Albaneze-Walker J;Leonard WR;Biba M;DaSilva J;Henderson D;Laing B;Mathre DJ;Spencer S;Bu XD .Adsorbent screening for metal impurity removal in pharmaceutical process research[J].Organic process research & development,2005(2):198-205. |
[4] | Zapf A;Beller M .[J].Topics in Catalysis,2002,19:101. |
[5] | Baumeister P;Meyer W;Oertle K;Seifert G Steiner H .[J].CHIMIA,1997,51:144. |
[6] | Blaser H U;Indolese A;Schnyder A;Steiner H Studer M .[J].Journal of Molecular Catalysis A:Chemical,2001,173:3. |
[7] | Zhao F;Bhanage B M;Shirai M;Arai M .[J].Chemistry-A European Journal,2000,6:843. |
[8] | Hagiwara H;Shimizu Y;Hoshi T;Suzuki T Ando M Okubo K Yokoyama C .[J].Tetrahedron Letters,2001,42:4349. |
[9] | Toebes ML.;de Jong YP.;van Dillen JA. .Synthesis of supported palladium catalysts [Review][J].Journal of molecular catalysis, A. Chemical,2001(1/2):75-98. |
[10] | Mehnert CP.;Ying JY.;Weaver DW. .Heterogeneous Heck catalysis with palladium-grafted molecular sieves[J].Journal of the American Chemical Society,1998(47):12289-12296. |
[11] | Djakovitch L;Koehler K .[J].Journal of the American Chemical Society,2001,123:5990. |
[12] | Djakovitch L;Koehler K .[J].Journal of Molecular Catalysis A:Chemical,1999,142:275. |
[13] | Biffis A;Zecca M;Basato M.[J].European Journal of Inorganic Chemistry,2011:1131. |
[14] | Wagner M;K?hler K;Djakovitch L;Weinkauf S Hagen V Muhler M .[J].Topics in Catalysis,2000,13:319. |
[15] | K?hler K;Wagner M;Djakovitch L .[J].Catalysis Today,2001,66:105. |
[16] | Li J;Mau A W H;Strauss C R.[J].Chemistry Communications,1997:1275. |
[17] | Zhang M;Guan J;Zhang B;Su D Williams C T Liang C .[J].Catalysis Letters,2012,142:313. |
[18] | Djakovitch L;Wagner M;Hartung C G;Beller M Koehler K .[J].Journal of Molecular Catalysis A:Chemical,2004,219:121. |
[19] | Corain B;Zecca M;Canton P;Centomo P .[J].Phil Trans R Soc A,2010,368:1495. |
[20] | Seki T;Grunwaldt J D;Baiker A.[J].Chemistry Communications,2007:3562. |
[21] | Seki T;Grunwaldt J D;van Vegten N;Baiker A .[J].Advanced Synthesis and Catalysis,2008,350:691. |
[22] | Laufer W;Hoelderich W F.[J].Chemistry Communications,2002:1684. |
[23] | Laufer W;Niederer J P M;Hoelderich W F .[J].Advanced Synthesis and Catalysis,2002,344:1084. |
[24] | Roveda A.;Benedetti A.;Pinna F.;Strukul G. .Palladium-tin catalysts on acrylic resins for the selective hydrogenation of nitrate[J].Inorganica Chimica Acta,2003(0):203-208. |
[25] | Gasparovicova D;Kralik M;Hronec M;Biffis A Zecca M Corain B .[J].Journal of Molecular Catalysis A:Chemical,2006,244:258. |
[26] | Xiang D;Liu X F;Sun J S;Xiao F S Sun J M .[J].Catalysis Today,2009,148:383. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%