欢迎登录材料期刊网

材料期刊网

高级检索

以基于借氢策略的苯甲醇和苯胺一步合成N-苯基苄胺为模型反应,研究了三种不同表面结构的氧化铝对其负载的Pt-Sn催化剂上N-烷基化合成仲胺反应性能的影响.采用N2吸附-脱附法、压汞法、X射线衍射、透射电镜、扫描电镜、CO脉冲吸附、H2-程序升温还原及NH3-程序升温脱附等技术对载体和Pt-Sn/Al2O3催化剂进行了表征.结果表明,与Al2O3相互作用较弱且高度分散的Pt颗粒具有很高的催化活性,Al2O3载体较大的孔体积和大孔分布的孔结构有助于反应物扩散和吸附到催化剂表面并提高反应活性.同时也有利于反应产物从催化剂表面离开,从而提高催化剂的稳定性.然而Al2O3较强的酸性及酸性分布降低了产物仲胺的选择性和催化剂稳定性.

参考文献

[1] Lawrence S A.Amines:Synthesis Properties and Applications[M].Cambridge:Cambridge University Press,2004
[2] Maiti, D;Buchwald, SL .Orthogonal Cu- and Pd-Based Catalyst Systems for the O- and N-Arylation of Aminophenols[J].Journal of the American Chemical Society,2009(47):17423-17429.
[3] Pahadi, NK;Paley, M;Jana, R;Waetzig, SR;Tunge, JA .Formation of N-Alkylpyrroles via Intermolecular Redox Amination[J].Journal of the American Chemical Society,2009(46):16626-16627.
[4] Klussmann M .[J].Angewandte Chemie International Edition,2009,48:7124.
[5] Marquard S L;Rosenfeld D C;Hartwig J F .[J].Angewandte Chemie International Edition,2010,49:793.
[6] Hamid MHSA;Slatford PA;Williams JMJ .Borrowing hydrogen in the activation of alcohols[J].Advanced synthesis & catalysis,2007(10):1555-1575.
[7] Hamid, MHSA;Allen, CL;Lamb, GW;Maxwell, AC;Maytum, HC;Watson, AJA;Williams, JMJ .Ruthenium-Catalyzed N-Alkylation of Amines and Sulfonamides Using Borrowing Hydrogen Methodology[J].Journal of the American Chemical Society,2009(5):1766-1774.
[8] Shiraishi Y;Sugano Y;Tanaka S;Hirai T .[J].Angewandte Chemie International Edition,2010,49:1656.
[9] Yamaguchi, K.;He, J.;Oishi, T.;Mizuno, N. .The "borrowing hydrogen strategy" by supported ruthenium hydroxide catalysts: Synthetic scope of symmetrically and unsymmetrically substituted amines[J].Chemistry: A European journal,2010(24):7199-7207.
[10] Grigg R;Mitchell T R B;Sutthivaiyakit S;Tongpenyai T.[J].Journal of the Chemical Society,Chemical Communications,1981:611.
[11] Yamaguchi R;Kawagoe S;Asai C;Fujita KI .Selective synthesis of secondary and tertiary amines by Cp*iridium-catalyzed multialkylation of ammonium salts with alcohols[J].Organic letters,2008(2):181-184.
[12] Pratt E F;Frazza E J .[J].Journal of the American Chemical Society,1954,76:6174.
[13] Shi F;Tse M K;Cui X J;G(o)rdes D Michalik D Thurow K Deng Y Q Beller M .[J].Angewandte Chemie International Edition,2009,48:5912.
[14] 赫巍,何松波,孙承林,吴凯凯,王连弟,余正坤.多相双金属Pt-Sn/γ-Al2O3催化的胺N-烷基化反应合成仲胺和叔胺[J].催化学报,2012(04):717-722.
[15] He, W.;Wang, L.;Sun, C.;Wu, K.;He, S.;Chen, J.;Wu, P.;Yu, Z. .Pt-Sn/γ-Al_2O_3-catalyzed highly efficient direct synthesis of secondary and tertiary amines and imines[J].Chemistry: A European journal,2011(47):13308-13317.
[16] Wang L D;He W;Wu K K;He S B Sun C L Yu Z K .[J].Tetrahedron Letters,2011,52:7103.
[17] He S B;Sun C L;Bai Z W;Dai X H Wang B .[J].Applied Catalysis A:General,2009,356:88.
[18] Casella ML.;Santori GF.;Ferretti OA.;Ramirez-Corredores MM.;Siri GJ. .Surface characterization of Li-modified platinum/tin catalysts for isobutane dehydrogenation[J].Langmuir: The ACS Journal of Surfaces and Colloids,2000(13):5639-5643.
[19] Carvalho L S;Pieck C L;Rangel M C;Figoli N S Grau J M Reyes P Parera J M .[J].Applied Catalysis A:General,2004,269:91.
[20] Afonso J C;Aranda D A G;Schmal M;Frety R .[J].Fuel Processing Technology,1995,42:3.
[21] Narayanan S;Sultana A;Le Q T;Auroux A .[J].Applied Catalysis A:General,1998,168:373.
[22] 张海,刘英,张勋高.碳包铁负载纳米钯催化苯甲醇选择氧化[J].催化学报,2011(11):1693-1701.
[23] 李丕高.微波辐射下苄醇直接脱水合成苄醚[J].石油化工,2007(05):489-491.
[24] 刘师 .[D].天津:天津大学,2001.
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:
  • 1
    0%
  • 2
    0%
  • 3
    0%
  • 4
    0%
  • 5
    0%