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Chemical looping reforming of biomass based pyrolysis gas coupling with chemical looping hydrogen by using Fe/Ni/Al oxygen carriers derived from LDH precursors

机译:使用源自LDH前体的Fe / Ni / Al氧载体,对基于生物质的热解气与化学环化氢进行化学环化重整

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Chemical looping reforming (CLR) coupling with chemical looping hydrogen (CLH) was proposed to reform biomass based pyrolysis gas and achieve high purity H-2 by using Fe/Ni/Al oxygen carriers derived from layered double hydroxide (LDH) precursors. The crystal form, morphology and reactivity of oxygen carriers were characterized by various analysis methods. The chemical looping reaction process was investigated in a fixed bed reactor. The experimental results exhibited that Fe0,99Ni0.6Al1.1O4 high dispersed oxygen carrier was synthesized. Moderate lattice oxygen releasing rate 0.00175 wt%/s and escape ratio 95.14% were achieved by the mixed oxygen carrier with Fe/Ni ratio of 3/1. Ni had positive effect on lattice oxygen escape ratio of oxygen carrier while Fe contributed to improve the instantaneous lattice oxygen releasing rate. Furthermore, the CH4/CO2 in biomass based pyrolysis gas was eliminated via CLR process based on the metal catalytic effect of oxygen carrier. The highest CH4 conversion 98.26% and CO2 conversion 71.92% were obtained in CLR process accompanying with the reduction of Fe0.99Ni0.6Al1.1O4 to Fe/Ni alloy. Additionally, H-2 with 96.56% purity was achieved in CLH process with the conversion of Fe/Ni alloy to Fe3O4. The H-2 instantaneous generation rate increased sharply to the maximum value 34.70 ml/min and then declined gradually. Ni0.6Fe2.4Al1.1O4 new high dispersed compound was generated in the regeneration stage with similar structure to fresh sample and more active Fe species content. Though the particle size of oxygen carrier tended to decline after whole reaction process, the porous structure was still reserved.
机译:提出了将化学环重整(CLR)与化学环重氢(CLH)耦合以重整生物质基热解气,并通过使用衍生自层状双氢氧化物(LDH)前体的Fe / Ni / Al氧载体实现高纯度H-2的方法。用各种分析方法表征了氧载体的晶形,形态和反应活性。在固定床反应器中研究了化学环化反应过程。实验结果表明,合成了Fe0,99Ni0.6Al1.1O4高分散氧载体。通过Fe / Ni比为3/1的混合氧载体实现了适度的晶格氧释放速率0.00175 wt%/ s和逸出率95.14%。 Ni对氧载体的晶格氧逸出率有积极影响,而Fe对提高瞬时晶格氧释放速率有积极作用。此外,基于氧气载体的金属催化作用,通过CLR工艺消除了基于生物质的热解气中的CH4 / CO2。随着Fe0.99Ni0.6Al1.1O4还原为Fe / Ni合金,CLR工艺获得了最高的CH4转化率98.26%和CO2转化率71.92%。此外,通过将Fe / Ni合金转化为Fe3O4在CLH工艺中获得了纯度为96.56%的H-2。 H-2瞬时产生速率急剧增加至最大值34.70 ml / min,然后逐渐下降。 Ni0.6Fe2.4Al1.1O4在再生阶段生成了新的高分散化合物,其结构与新鲜样品相似,并且具有更多的活性铁。尽管在整个反应过程后氧载体的粒径趋于减小,但仍保留了多孔结构。

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