Pristine ETS-10 and AM-6 and their Co2+-exchanged forms were prepared, and their catalytic activi-ties toward the oxidation of styrene in oxygen atmosphere were studied in dimethylformamide. The catalysts were denoted as Co-E10-n (n=0, 9, 26, 68, 81) and Co-A6-m (m=0, 8, 23, 63, 79), where n and m denote the degree of Co2+exchange. The products of the oxidation process were identified as styrene epoxide (E) and benzaldehyde (B). Both the pristine forms, ETS-10 (Co-E10-0) and AM-6 (Co-A6-0), and Co2+-exchanged forms displayed catalytic activities. With increasing n or m, the con-version, and hence the rate, increased. Specifically, the rates varied from 6.1 to 12.5 mmol·g?1·h?1 with increasing n (Co-E10-n catalysts) and from 5.4 to 12.4 mmol·g?1·h?1 with increasing m (Co-A6-m catalysts). In contrast, the E/B ratio decreased with increasing n or m. More specifically, the E/B ratio decreased from 2.1 to 0.1 with increasing n from 0 to 81 (Co-E10-n catalysts) and from 1.3 to 0.1 with increasing m from 0 to 79 (Co-A6-m catalysts). Co-E10-9 displayed the highest E yield and Co-A6-79 generated the highest B yield. The highest turnover frequency obtained was 36.3 Co?1·h?1, which was the highest one obtained among those obtained for the Co2+-exchanged zeolites and mesoporous silica reference materials studied in this work.
参考文献
[1] | Joergensen K A .[J].CHEMICAL REVIEWS,1989,89:431. |
[2] | Neumann R;Dahan M .[J].NATURE,1997,388:353. |
[3] | Hill C L .[J].NATURE,1999,401:436. |
[4] | Ishii Y;Sakaguchi S;Iwahama T .[J].Advanced Synthesis and Catalysis,2001,343:393. |
[5] | Tang Q H;Wang Y;Liang J;Wang P,Zhang Q H,Wan H L.[J].Chemistry Communications,2004:440. |
[6] | Tang Q H;Zhang Q H;Wu H L;Wang Y .[J].Journal of Catalysis,2005,230:384. |
[7] | Sebastian J;Jinka K M;Jasra R V .[J].Journal of Catalysis,2006,244:208. |
[8] | Patil M V;Yadav M K;Jasra R V .[J].Journal of Molecular Catalysis A:Chemical,2007,277:72. |
[9] | Jinka K M;Pai S M;Newalkar B L;Choudary N V Jasra R V .[J].CATALYSIS COMMUNICATIONS,2010,11:638. |
[10] | Cui H T;Zhang Y;Zhao L F;Zhu Y L .[J].CATALYSIS COMMUNICATIONS,2011,12:417. |
[11] | Xu G;Xia QH;Lu XH;Zhang Q;Zhan HJ .Selectively catalytic epoxidation of styrene with dry air over the composite catalysts of Co-ZSM-5 coordinated with ligands[J].Journal of molecular catalysis, A. Chemical,2007(1/2):180-187. |
[12] | Qi B;Lu X H;Fang S Y;Lei J,Dong Y L,Zhou D,Xia Q H .[J].Journal of Molecular Catalysis A:Chemical,2011,334:44. |
[13] | Tang B;Lu X H;Zhou D;Lei J Niu Z H Fan J Xia Q H .[J].CATALYSIS COMMUNICATIONS,2012,21:68. |
[14] | Tang B;Lu X H;Zhou D;Tian P Niu Z H Zhang J L Chen X Xia Q H .[J].CATALYSIS COMMUNICATIONS,2013,3:42. |
[15] | Zhou D;Tang B;Lu X H;Wei X L Li K Xia Q H .[J].CATALYSIS COMMUNICATIONS,2014,45:124. |
[16] | Wei X L;Lu X H;Ma X T;Peng C,Jiang H Z,Zhou D,Xia Q H .[J].CATALYSIS COMMUNICATIONS,2015,61:48. |
[17] | Kuznicki S M .[P].US Patent 4853202,1989. |
[18] | Anderson M W;Terasaki O;Ohsuna T;Philippou A MacKay S P Ferreira A Rocha J Lidin S .[J].NATURE,1994,367:347. |
[19] | Anderson M W;Terasaki O;Ohsuna T;Malley P J O Philippou A MacKay S P Ferreira A Rocha J Lidin S .[J].PHILOSOPHICAL MAGAZINE B-PHYSICS OF CONDENSED MATTER STATISTICAL MECHANIC,1995,71:813. |
[20] | Rocha J;Brandao P;Lin Z;Anderson M W Alfredsson V Terasaki O .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,1997,36:100. |
[21] | Datta S J;Yoon K B .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2010,49:4971. |
[22] | Datta, S.J.;Yoon, K.B. .Length-dependent change of optical, magnetic, and vibrational properties of vanadate (V ~(IV)O _3 ~(2-)) quantum wire embedded in AM-6 vanadosilicate[J].Journal of the American Chemical Society,2012(41):17202-17211. |
[23] | Jeong N C;Lee M H;Yoon K B .[J].ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2007,46:5868. |
[24] | Datta S J;Yoon K B .[J].Catalysis Today,2013,204:60. |
- 下载量()
- 访问量()
- 您的评分:
-
10%
-
20%
-
30%
-
40%
-
50%