B改性CuZnAlOx催化剂对甲醇水蒸气重整制氢性能的研究

Hydrogen production from methanol steam reforming over B-modified CuZnAlOx catalysts

    摘要
  • 摘要: 采用共沉淀法制备CuZnAlOx（CZA）催化剂，通过浸渍法得到一系列不同硼（B）负载量的yB/CZA（y=0.28%、0.38%、0.73%、0.89%和4.10%，质量分数）催化剂，并将其用于甲醇水蒸气重整制氢反应。此外，为探究催化剂的构效关系，采用ICP、BET、SEM、N2O化学吸附、TEM、XRD、H2-TPR和XPS等手段对催化剂进行表征。结果表明，B引入主要影响催化剂的Cu分散性、还原性及Cu-B间相互作用，进而影响甲醇水蒸气重整制氢性能。其中，0.38B/CZA催化剂获得最高催化活性，这与其具有较高的Cu分散性与较强的Cu-B相互作用力有关；在反应温度为250℃，n（H2O）：n（CH3OH）=3，空速为9000 mL/（g·h）时，CH3OH转化率达到93%，CO选择性仅有0.3%，且反应102 h后仍未失活。

     

    Abstract: In this work, CuZnAlOx (CZA) catalysts prepared by coprecipitation method and a series of yB/CZA catalysts with various boron loadings (y=0.28%, 0.38%, 0.73%, 0.89% and 4.10%) prepared by impregnation method were used in the methanol steam reforming for hydrogen production. In addition, the B-modified CZA catalysts were deeply characterized by different techniques such as ICP, BET, SEM, N2O chemisorption, TEM, XRD, H2-TPR and XPS to explore the structure-activity relationship. The characterization results revealed that the introduction primarily affected the Cu dispersion, reductibility and the interaction between the boron and copper species. The 0.38B/CZA catalyst revealed the optimum catalytic performance among the researched catalysts, which were due to the presence of highly dispersed Cu particles and the strong interaction between the boron and copper species. The 93% methanol conversion, the CO selectivity as low as 0.3%, and the long-time stability with 102 h time on stream were obtained over it when the reaction conditions were 250℃, n(H2O):n(CH3OH)=3 and GHSV=9000 mL/(g·h).

     

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