研究了非负载型铁催化剂上CO2加氢制低碳烯烃反应.结果显示,添加碱金属可显著提高铁催化剂上的CO2转化率和烯烃选择性.在经K和Rb修饰的Fe催化剂上,CO2转化率可达约40%,烯烃选择性达到50%以上,其中C2~C4烯烃收率超过10%.催化剂表征结果表明,碱金属促进了催化剂中碳化铁的生成,这可能是催化剂性能提高的一个关键原因.随着K含量由1wt%增加至5wt%,CO2转化率及烯烃选择性均升高.但K含量过高时,催化剂活性降低.这可能是由于催化剂比表面积和CO2化学吸附量降低所致.当K含量为5%~10%时,K-Fe催化剂上烯烃收率较高;进一步添加适量的硼可进一步提高烯烃选择性,且CO2转化率下降不大.
参考文献
[1] | Baiker A .[J].Applied Organometallic Chemistry,2000,14:751. |
[2] | Song C S .[J].Catalysis Today,2006,115:2. |
[3] | Ma J;Sun N N;Zhang X L;Zhao N Xiao F K Wei W Sun Y H .[J].Catalysis Today,2009,148:221. |
[4] | 靳治良,钱玲,吕功煊.二氧化碳化学--现状及展望[J].化学进展,2010(06):1102-1115. |
[5] | Wang W;Wang Sh P;Ma X B;Gong J L .[J].CHEMICAL SOCIETY REVIEWS,2011,40:3703. |
[6] | 王丹君,陶芙蓉,赵华华,宋焕玲,丑凌军.CO2辅助老化制备的Cu/ZnO/Al2O3催化剂上CO2加氢制甲醇[J].催化学报,2011(09):1452-1456. |
[7] | Feyzi M;Hassankhani A .[J].Journal of Natural Gas Chemistry,2011,20:677. |
[8] | Lu J Y;Liu Y C;Li N .[J].Journal of Natural Gas Chemistry,2011,20:423. |
[9] | Prasad P S S;Bae J W;Jun K-W;Lee K-W .[J].CATALYSIS SURVEYS FROM ASIA,2008,12:170. |
[10] | Fujimoto K;Shikada T .[J].Applied Catalysis,1987,31:13. |
[11] | Cubeiro M L;Valderrama G;Goldwasser M R;González-Jiménez F da Silva M C Pérez-Zurita M J .[J].Studies in surface science and catalysis,1997,107:231. |
[12] | Riedel T;Schaub G;Jun K-W;Lee K-W .[J].Ind gng Chem Res,2001,40:1355. |
[13] | Zhang Q H;gang J C;Wang Y .[J].ChemCatChem,2010,2:1030. |
[14] | de Smit E;Weckhuysen B M .[J].CHEMICAL SOCIETY REVIEWS,2008,37:2758. |
[15] | Choi P H;Jun K-W;Lee S-J;Choi M-J Lee K-W .[J].Catalysis Letters,1996,40:115. |
[16] | Dorner R W;Hardy D R;Williams F W;Willauer H D .[J].CATALYSIS COMMUNICATIONS,2011,15:88. |
[17] | Kim J-S;Lee S;Lee S-B;Choi M-J Lee K-W .[J].Catalysis Today,2006,115:228. |
[18] | Kishan M;Lee M-W;Nam S-S;Choi M-J Lee K-W .[J].Catalysis Letters,1998,56:215. |
[19] | Lee S-C;Jang J-H;Lee B-Y;Kang M-C Kang M Choung S-J .[J].Applied Catalysis A:General,2003,253:293. |
[20] | Xu L-Y;Wang Q X;Liang D B;Wang X Lin L W Cui W Xu Y D .[J].Applied Catalysis A:General,1998,173:19. |
[21] | Herranz T;Rojas S;Perez-Alonso FJ;Ojeda A;Terreros P;Fierro JLG .Hydrogenation of carbon oxides over promoted Fe-Mn catalysts prepared by the microemulsion methodology[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2006(0):66-75. |
[22] | Yang, C.;Zhao, H.;Hou, Y.;Ma, D. .Fe _5C _2 nanoparticles: A facile bromide-induced synthesis and as an active phase for Fischer-Tropsch synthesis[J].Journal of the American Chemical Society,2012(38):15814-15821. |
[23] | Dorner R W;Hardy D R;Williams F W;Willauer H D .[J].Applied Catalysis A:General,2010,373:112. |
[24] | Brainard W A;Wheeler D R .[J].Journal of Vacuum Science and Technology,1978,15:1800. |
[25] | Yu G B;Sun B;Pei Y;Xie S H Yah S R Qiao M H Fan K N Zhang X X Zong B N .[J].Journal of the American Chemical Society,2010,132:935. |
[26] | De Smit, E.;Cinquini, F.;Beale, A.M.;Safonova, O.V.;Van Beek, W.;Sautet, P.;Weckhuysen, B.M. .Stability and reactivity of ε-Χ-θ iron carbide catalyst phases in fischer-tropsch synthesis: Controlling μ_c[J].Journal of the American Chemical Society,2010(42):14928-14941. |
[27] | Li J;Coville N J .[J].Applied Catalysis A:General,1999,181:201. |
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