在NH_4OAc和HOAc的促进下,使用环境友好的丙酮-水混合溶剂,六齿八羟基喹啉锰类配合物(Q_3Mn~Ⅲ)能够高效地催化H_2O_2氧化二甲亚砜(DMSO).卤素取代的Q_3Mn~Ⅲ配合物具有更高的催化活性,这归因于卤索取代基能加强Q_3Mn~Ⅲ的畸变效应,这一点经B3LYP/6.311G+(d)计算得到证实.另外考察了一些因素对反应的影响,并提出了一个催化反应机理.
A series of hexadentate 8-quinolinolato manganese(III) complexes (Q_3Mn~III), with NH4OAc and HO Ac as additives, were highly efficient catalysts for the oxidation of dimethylsulfoxide (DMSO) with aqueous hydrogen peroxide in an environmentally friendly acetone-water medium. The halogen substituents on the ligand improved the catalytic efficiency of Q_3Mn~III complexes, which was likely due to their strong distortion effect on Q_3Mn~III as indicated by the B3LYP/6-311 G+(d) calculation. Various parameters were investigated and a reaction mechanism was proposed.
参考文献
[1] | 徐兆瑜 .[J].化工中间体,2002,21(09) |
[2] | 蒋朝哲,阳海,许冠兵,郭鹏.微波辐射下4A分子筛催化γ-内酰胺的合成及用粗糙集理论进行溶剂筛选[J].催化学报,2005(04):263-264. |
[3] | Maciuca A L;Dumitriu E;Francois F;Hulea V .[J].CHEMOSPHERE,2007,68:227. |
[4] | Park S J;Yoon T I;Bae J H;Seo H J,Park H J .[J].Process Biochemistry,2001,36:579. |
[5] | Budavari S;O'Neil M J;Smith A;Heckelman P E.The Merk Index[M].New Jersey:Merk & Co,1989:962. |
[6] | Pereira-Ramos J P;Messina R;Perichon J .[J].Journal of Applied Electrochemistry,1986,16:379. |
[7] | Borodina E.;Rainey FA.;Ward-Rainey NL.;Wood AP.;Kelly DP. .Dimethylsulfone as a growth substrate for novel methylotrophic species of Hyphomicrobium and Arthrobacter[J].Archives of microbiology,2000(5/6):425-437. |
[8] | 孔令艳,李钢,王祥生,王云.TS-1/过氧化氢催化体系中有机硫化物的选择氧化[J].催化学报,2004(10):775-778. |
[9] | Wu J J;Muruganandham M;Yang J S;Lin S S .[J].Catalysis Communications,2006,7:901. |
[10] | Zhong S;Tan YM;Fu ZH;Me QJ;Xie F;Zhou XP;Ye ZP;Peng GS;Yin DL .A highly efficient method of epoxidation of olefins with hydrogen peroxide catalyzed by changeable hexadentate 8-quinolinolato manganese(III) complexes[J].Journal of Catalysis,2008(1):154-158. |
[11] | Zhong S;Fu Z H;Tan Y M;Xie Q J Xie F Zhou X P Ye Z P Peng G S Yin D L .[J].Advanced Synthesis and Catalysis,2008,350:802. |
[12] | Ye ZP;Fu ZH;Zhong S;Xie F;Zhou XP;Liu FL;Yin DL .Selective oxidation of alcohols with hydrogen peroxide catalyzed by hexadentate binding 8-quinolinolato manganese(III) complexes[J].Journal of Catalysis,2009(1):110-115. |
[13] | Renaud J P;Battioni P;Bartoli J F;Mansuy D.[J].Journal of the Chemical Society,Chemical Communications,1985:888. |
[14] | Crawford S M .[J].Spectrochimica Acta,1963,19:255. |
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