采用化学还原法在纯水中制备了纳米铁基催化剂,将其直接分散到液态聚乙二醇(PEG)中进行费托合成(FTS)反应.透射电子显微镜、X射线衍射、穆斯堡尔谱和X射线光电子能谱等结果表明,还原态催化剂粒径在30～65 nm,主要由无定彤的Fe-B和a-Fe组成,其中B部分电子向Fe转移.反应过程中,无定形的Fe-B首先快速转变为α-Fe,而α-Fe很容易发生碳化或氧化,最终转变为Fe3O4和碳化铁.PEG能有效抑制纳米粒子的聚集长大,反应后催化剂粒径减小为20～55nm.在3.0MPa,V(H2)/V(CO)=2和200℃的反应条件下,该催化剂表现出优异的FTS低温活性和较高的稳定性,反应后产物和催化体系很容易实现分离.
参考文献
| [1] | Adesina A A .[J].Applied Catalysis A:General,1996,138:345. |
| [2] | Schulz H .[J].Applied Catalysis A:General,1999,186:3. |
| [3] | Espinoza R L;Steynberg A P;Jager B;Vosloo A C .[J].Applied Catalysis A:General,1999,186:13. |
| [4] | 寇元,何玲.离子液体与绿色化学：为了今天还是为了未来?[J].化学进展,2008(01):5-10. |
| [5] | 寇元.合成气催化转化的绿色化学[J].催化学报,2008(09):817-822. |
| [6] | 杨咏来,徐恒泳,李文钊.纳米粒子催化剂及其研究进展[J].材料导报,2003(02):12-14. |
| [7] | Astruc D;Lu F;Aranzaes J R .[J].Angewandte Chemie International Edition,2005,44:7852. |
| [8] | Schl6gl R;Hamid S B A .[J].Angewandte Chemie International Edition,2004,43:1628. |
| [9] | Saib A M;Borgna A;van de Loosdrecht J;van Berge P J,Geus J W,Niemantsverdriet J W .[J].Journal of Catalysis,2006,239:326. |
| [10] | Choi H;Al-Abed S R;Agarwal S;Dionysiou D D .[J].Chemistry of Materials,2008,20:3649. |
| [11] | Chen, W;Fan, ZL;Pan, XL;Bao, XH .Effect of confinement in carbon nanotubes on the activity of Fischer-Tropsch iron catalyst[J].Journal of the American Chemical Society,2008(29):9414-9419. |
| [12] | Ott L S;Finke R G .[J].Coordination Chemistry Reviews,2007,251:1075. |
| [13] | Lee JH;Cha KE;Kim MS;Hong HW;Chung DJ;Ryu G;Myung H .Nanosized polyamidoamine (PAMAM) dendrimer-induced apoptosis mediated by mitochondrial dysfunction.[J].Toxicology Letters,2009(2):202-207. |
| [14] | Chauhan B P S;Rathore J S .[J].Bandoo T J Am Chem Soc,2004,126:8493. |
| [15] | Xiao C X;Wang H Z;Mu X D;Kou Y .[J].Journal of Catalysis,2007,250:25. |
| [16] | Salavati;Niasari M.Fereshteh Z,Davar F .[J].POLYHEDRON,2009,28:126. |
| [17] | Widegren JA.;Finke RG. .Anisole hydrogenation with well-characterized polyoxoanion- and tetrabutylammonium-stabilized Rh(0) nanoclusters: Effects of added water and acid, plus enhanced catalytic rate, lifetime, and partial hydrogenation selectivity[J].Inorganic Chemistry: A Research Journal that Includes Bioinorganic, Catalytic, Organometallic, Solid-State, and Synthetic Chemistry and Reaction Dynamics,2002(6):1558-1572. |
| [18] | Liu SF;Xiao JL .Toward green catalytic synthesis - Transition metal-catalyzed reactions in non-conventional media[J].Journal of molecular catalysis, A. Chemical,2007(1/2):1-43. |
| [19] | Hornstein BJ.;Finke RG. .Transition-metal nanocluster catalysts: Scaled-up synthesis, characterization, storage conditions, stability, and catalytic activity before and after storage of polyoxoanion- and tetrabutylammonium-stabilized Ir(0) nanoclusters [Review][J].Chemistry of Materials,2003(4):899-909. |
| [20] | Schulz J;Roucoux A;Patin H.[J].Chemistry Communications,1999:535. |
| [21] | Xiao C X;Cai Z P Wang T;Kou Y;Yah N .[J].Angewandte Chemie International Edition,2008,47:746. |
| [22] | Silva D O;Scholten J D;Gelesky M A;Teixeira S R,Dos Santos A C B,Souza-Aguiar E F Dupont J .[J].ChemSusChem,2008,1:291. |
| [23] | Scariot M;Silva D O;Scholten J D;Machado G Teixeira S R,Novak M A,Ebeling G'Dupont J .[J].Angewandte Chemie International Edition,2008,47:9075. |
| [24] | Mahajan D;Kobayashi A;Gupta N.[J].Chemistry Communications,1994:795. |
| [25] | 吴宝山,田磊,白亮,张志新,相宏伟,李永旺.沉淀铁催化剂在F-T合成中的研究与应用进展[J].化学进展,2004(02):256-265. |
| [26] | Chandrasekhar S;Reddy G P K;Nagesh C;Reddy C R .[J].Tetrahedron Letters,2007,48:1269. |
| [27] | Chandrasekhar S;Reddy NR;Sultana SS;Narsihmulu C;Reddy KV .L-Proline catalysed asymmetric aldol reactions in PEG-400 as recyclable medium and transfer aldol reactions[J].Tetrahedron,2006(2/3):338-345. |
| [28] | Sun YP;Li XQ;Cao JS;Zhang WX;Wang HP .Characterization of zero-valent iron nanoparticles[J].Advances in colloid and interface science,2006(1/3):47-56. |
| [29] | Zhu Y;Liu F P;Ding W P;Guo X F Chen Y .[J].Angewandte Chemie International Edition,2006,45:7211. |
| [30] | Bafinov V A;Tsurin V A;Voronin V I;Novikov S I,Sufikov V T .[J].The Physics of Metals and Metallography,2006,101:456. |
| [31] | Balogh J;Bujdoso L;Kemeny T;Vincze I .[J].Journal of Physics:Condensed Matter,1997,9:L503. |
| [32] | Suo Z H;Kou Y Niu J Z;Zhang W Z;Wang H L .[J].Applied Catalysis A:General,1997,148:301. |
| [33] | Martino A;Stoker M;Hicks M;Bartholomew C H,Sault A G Kawola J S .[J].Applied Catalysis A:General,1997,161:235. |
| [34] | An X;Wu B S;Hou W J;Wan H J,Tao Z C,Li T Z,Zhang Z X,Xiang H W,Li Y W,Xu B F,Yi F .[J].Applied Catalysis A:General,2007,263:266. |
| [35] | Li H;Liu J;Xie SH;Qiao MH;Dai WL;Li HX .Highly active Co-B amorphous alloy catalyst with uniform nanoparticles prepared in oil-in-water microemulsion[J].Journal of Catalysis,2008(1):104-110. |
| [36] | de Smit E;Weckhuysen B M .[J].Chemical Society Reviews,2008,37:2758. |
| [37] | Tavakoli A;Sohrabi M;Kargari A .[J].Chemical Engineering Journal,2008,136:358. |
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