Characterization and evaluation of Ni/SiO2 catalysts for hydrogen production and tar reduction from catalytic steam pyrolysis-reforming of refuse derived fuel

Characterization and evaluation of Ni/SiO2 catalysts for hydrogen production and tar reduction from catalytic steam pyrolysis-reforming of refuse derived fuel
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DOI:
10.1016/j.apcatb.2013.01.016
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发表时间:
2013-05-02
影响因子:
22.1
通讯作者:
Williams, Paul T.
Williams, Paul T.
中科院分区:
化学1区
文献类型:
--
作者:
Blanco, Paula H.;Wu, Chunfei;Williams, Paul T.

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以垃圾衍生燃料(RDF)为原料,制备了一系列Ni/SiO_2催化剂,考察了它们在两段热解-重整系统中制氢降焦的适用性。实验在600℃的热解温度和800℃的重整温度下进行,产物气体用气相色谱(GC)分析,缩合组份用气相色谱-质谱仪(GC-MS)测定。考察了催化剂的制备方法、镍含量以及金属助剂(Ce、Mg、Al)的添加对催化剂性能的影响。采用BET比表面积分析、程序升温氧化(TPO)和扫描电子显微镜(SEM)对催化剂进行了表征。TPO和扫描电子显微镜分析表明,浸渍法制备的Ni/SiO_2催化剂倾向于沉积无定形碳,而溶胶-凝胶法制备的催化剂倾向于沉积丝状炭。添加金属助剂(Ce、Mg、Al)对溶胶-凝胶法制备的Ni/SiO_2催化剂的氢产率和焦油生成量的影响不大。用Sol-Gel法制备的20wt.%Ni/SiO_2催化剂,氢气浓度最高可达57.9%,焦油生成量最低为0.24 mg(TAR)/g(RDF);另一方面,浸渍系列催化剂对H-2的催化活性较低,焦油生成量较高,这可能是由于催化剂的比表面积和孔径较小,以及催化剂表面形成无定形碳所致。在分析的焦油样品中主要发现了烯烃和醇的官能团,其中主要的含量是苯乙烯、苯酚、吲哚、甲酚、萘、荧和菲。(C)2013爱思唯尔B.V.保留所有权利。
A series of Ni/SiO2 catalysts have been prepared and investigated for their suitability for hydrogen production and tar reduction in a two-stage pyrolysis-reforming system, using refuse derived fuel (RDF) as the raw material. Experiments were conducted at a pyrolysis temperature of 600 degrees C, and a reforming temperature of 800 degrees C. The product gases were analysed by gas chromatography (GC) and the condensed fraction was collected and quantified using gas chromatography-mass spectrometry (GC-MS). The effects of the catalyst preparation method, nickel content and the addition of metal promoters (Ce, Mg, Al), were investigated. Catalysts were characterised using BET surface area analysis, temperature programmed oxidation (TPO), and scanning electron microscopy (SEM). The TPO and SEM analysis of the reacted catalysts showed that amorphous type carbons tended to be deposited over the Ni/SiO2 catalysts prepared by impregnation, while filamentous type carbons were favoured with the sol-gel prepared catalysts. The influence of catalyst promoters (Ce, Mg, Al) added to the Ni/SiO2 catalyst prepared by the sol-gel method was found not to be significant, as the H-2 production was not increased and the tar formation was not reduced with the metal-added catalyst. The highest H-2 concentration of 57.9 vol.% and lower tar amount produced of 0.24 mg(tar)/g(RDF); were obtained using the 20 wt.% Ni/SiO2 catalyst prepared by sol-gel. On the other hand a low catalytic activity for H-2 production and higher tar produced were found for the impregnated series of catalysts, which might be due to the smaller surface area, pore size and due to the formation of amorphous carbons on the catalyst surface. Alkenes and alcohol functional groups were mainly found in the analysed tar samples, with major concentrations of styrene, phenol, indene, cresols, naphthalene, fluorene, and phenanthrene. (C) 2013 Elsevier B.V. All rights reserved.