二甲醚部分氧化重整制氢催化剂作用的研究
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摘要
通过对比催化剂不同搭配方式,分析讨论了二甲醚(DME)分解反应和部分氧化重整反应中催化剂所起的作用。DME在高温下容易直接分解生成CH_4、CO和H_2。Pt/Al_2O_3催化剂会促进DME分解生成CH_3O和CH_3自由基,提高H_2收率,但对CO和CH_4的影响不大。Ni/Al_2O_3催化剂主要催化CH_4与H_2O或CO_2重整反应,从而减少CH_4的生成。在DME部分氧化反应中,DME会发生深度氧化反应生成CO_2与H_2O,同时伴随着DME直接分解反应。Pt/Al_2O_3催化剂在一定程度上会抑制DME的分解,起到了催化部分氧化反应的作用,也能催化CH_4与H_2O或CO_2的重整反应。Ni/Al_2O_3则主要发挥了催化CH_4与H_2O或CO_2重整反应的作用。
In this paper, the roles of catalysts in hydrogen production from partial oxidation and reforming of dimethyl ether(DME) were investigated by comparing the reaction performance with different catalysts loading manners. At high temperature, DME is easy to be decomposed to give CH_4, CO and H_2. Pt/Al_2O_3 catalyst can promote the decomposition of DME to CH_3O and CH_3 free radicals, so as to increase H_2 yield. But it gives little effect on the production of CO and CH_4. Ni/Al_2O_3 catalyst takes the effect of reforming CH_4 with H_2O or CO_2, so as to decrease the production of CH_4. In the partial oxidation and reforming of DME, deep oxidation of DME takes place accompanied by direct decomposition. Pt/Al_2O_3 catalyst can inhibit the decomposition and promote partial oxidation of DME, and it can promote the reforming of CH_4 with H_2O or CO_2. Ni/Al_2O_3 catalyst mainly takes the catalytic effect on the reforming of CH_4 with H_2O or CO_2.
In this paper, the roles of catalysts in hydrogen production from partial oxidation and reforming of dimethyl ether(DME) were investigated by comparing the reaction performance with different catalysts loading manners. At high temperature, DME is easy to be decomposed to give CH_4, CO and H_2. Pt/Al_2O_3 catalyst can promote the decomposition of DME to CH_3O and CH_3 free radicals, so as to increase H_2 yield. But it gives little effect on the production of CO and CH_4. Ni/Al_2O_3 catalyst takes the effect of reforming CH_4 with H_2O or CO_2, so as to decrease the production of CH_4. In the partial oxidation and reforming of DME, deep oxidation of DME takes place accompanied by direct decomposition. Pt/Al_2O_3 catalyst can inhibit the decomposition and promote partial oxidation of DME, and it can promote the reforming of CH_4 with H_2O or CO_2. Ni/Al_2O_3 catalyst mainly takes the catalytic effect on the reforming of CH_4 with H_2O or CO_2.
引文
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[17]张启俭,杜凤,何欣欣,等.二甲醚部分氧化重整制氢部分氧化催化剂的考察[J].催化学报,2009,30(6):519-524.
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[19]Ma K,Li X.Hydrogen production from partial oxidation of DME by spark discharge plasma[J].Fuel Chem Techn,2011,39(11):844-84.
[2]Takeishi K,Suzuki H.Steam reforming of DME[J].Appl Catal A:Gen,2004,260(1):111-117.
[3]Yamada Y,Mathew T,Ueda A,et al.A novel DME steam-reforming catalyst designed with fact database on-demand[J].Appl Surf Science,2006,252(7):2593-2597.
[4]Feng D,Zuo Y,Wang D,et al.Steam Reforming of DME over Coupled ZSM-5 and Cu-Zn-Based Catalysts[J].Catal,2009,30(3):223-229.
[5]Wang X,Pan X,Lin R,et al.Steam reforming of DME over Cu-Ni/γ-Al2O3 bi-functional catalyst prepared by deposition-precipitation method[J].Hydrogen Energy,2010,35(9):4060-4068.
[6]Li J,Zhang Q,Long X,et al.Hydrogen production for fuel cells via steam reforming of DME over commercial Cu/Zn O/Al2O3 and zeolite[J].Chemical Engineering Journal,2012,187(1):299-305.
[7]Zhang L,Meng M,Zhou S,et al.Promotional effect of Partial substitution of Zn by Ce in Cu/Zn/Al2O3 catalysts used for hydrogen production via steam reforming of DME[J].Power Sources,2013,232(15):286-296.
[8]寇素原,王晓蕾,任克威.二甲醚水蒸气重整制氢过程的热力学分析[J].天然气化工,2009,34(1):35-40.
[9]Wang S,Ishihara T,Takita Y.Partial oxidation of DME over various supported metal catalysts[J].Appl Catal A:Gen,2002,228(1-2):167-176.
[10]Zhang Q,Li X,Fujimoto K,et al.Hydrogen production by partial oxidation and reforming of DME[J].Appl Catal A:Gen l,2005,288(1-2):169-174.
[11]Zhang Q,Li X,Fujimoto K,et al.Hydrogen production from partial oxidation and reforming of DME[J].Catal Lett,2005,102(3-4):197-200.
[12]李聪,李兴虎,姜磊,等.二甲醚部分氧化重整制氢的研究[J].武汉理工大学学报,2006,28(专辑II):159-163.
[13]李聪,李兴虎,姜磊,等.二甲醚部分氧化重整的参数优化与动力学[J].电源技术,2007,31(10):779-781.
[14]宋凌珺,李兴虎,李聪,等.二甲醚部分氧化重整制氢的实验研究[J].燃料化学学报,2008,36(1):16-19.
[15]Chen Y,Shao Z,Xu N.Partial oxidation of DME to H2/syngas over supported Pt catalyst[J].Nat Gas Chem,2008,17(1):75-80.
[16]Zhang Q,Du F,He X,etal.Hydrogen production via partial oxidation and reforming of DME[J].Catal Today,2009,146(1-2):50-56.
[17]张启俭,杜凤,何欣欣,等.二甲醚部分氧化重整制氢部分氧化催化剂的考察[J].催化学报,2009,30(6):519-524.
[18]Zou J,Zhang Y,Liu C.Hydrogen production from partial oxidation of DME using corona discharge plasma[J].Hydrogen Energy,2007,32(8):958-964.
[19]Ma K,Li X.Hydrogen production from partial oxidation of DME by spark discharge plasma[J].Fuel Chem Techn,2011,39(11):844-84.