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多种金属掺杂的镍基催化剂用于中温重整生物油制氢的设计

Design of Multiple Metal Doped Ni Based Catalyst for Hydrogen Generation from Bio-oil Reforming at Mild-temperature

  • 摘要: 一种新的由共沉淀法合成的多种金属(铜、镁、铈)掺杂的镍基混合氧化物催化剂,在250~500 oC用于生物油高效重整制氢. 摩尔比为Ni:Cu:Mg:Ce:Al=5.6:1.1:1.9:1.0:9.9的催化剂表现出较高的催化重整活性,在传统的水蒸气重整模式和500 oC条件下,氢产率达82.8%;电催化重整模式中,在400 oC 和3.1 A,氢产率达91.1%.ECR模式中重整温度和通过催化剂电流促进生物油的重整和热裂解.另外催化剂在300~600 oC显示出较高的水煤气变化反应活性,生物油重整过程中催化剂性质的变化利用ICP、XRD、XPS和BET进行了表征. 生物油重整机理基于基元反应、催化剂表征进行了讨论.

     

    Abstract: A new kind of multiple metal (Cu, Mg, Ce) doped Ni based mixed oxide catalyst, synthesized by the co-precipitation method, was used for efficient production of hydrogen from bio-oil reforming at 250-500 oC. Two reforming processes, the conventional steam reforming (CSR) and the electrochemical catalytic reforming (ECR), were performed for the bio-oil reforming. The catalyst with an atomic mole ratio of Ni:Cu:Mg:Ce:Al=5.6:1.1:1.9:1.0:9.9 exhibited very high reforming activity both in CSR and ECR processes, reaching 82.8% hydrogen yield at 500 oC in the CSR, yield of 91.1% at 400 oC and 3.1 A in the ECR, respectively. The influences of reforming temperature and the current through the catalyst in the ECR were investigated. It was observed that the reforming and decomposition of the bio-oil were significantly enhanced by the current. The promoting effects of current on the decomposition and reforming processes of bio-oil were further studied by using the model compounds of bio-oil (acetic acid and ethanol) under 101 kPa or low pressure (0.1 Pa) through the time of flight analysis. The catalyst also shows high water gas shift activity in the range of 300-600 oC. The catalyst features and alterations in the bio-oil reforming were characterized by the ICP, XRD, XPS and BET measurements. The mechanism of bio-oil reforming was discussed based on the study of the elemental reactions and catalyst characterizations. The research catalyst, potentially, may be a practical catalyst for high efficient production of hydrogen from reforming of bio-oil at mild-temperature.

     

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