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    NiFeAlO4载氧体制备及煤化学链燃烧反应特性

    Synthesis of NiFeAlO_4 oxygen carrier and its coal chemical looping combustion performance

    • 摘要: 采用共沉淀法和溶胶凝胶法制备了具有尖晶石结构的NiFeAlO4载氧体,考察了制备方法、载氧体与煤质量比对NiFeAlO4载氧体化学链燃烧特性和循环稳定性的影响,并分析了载氧体对煤转化过程的作用。结果表明,溶胶凝胶法制备的NiFeAlO4载氧体具有更好的反应性,当载氧体与煤质量比为20:1时,碳转化率为86.7%,远高于煤单独热解时的碳转化率(34%),此时CO2浓度为93.6%。对反应前后NiFeAlO4载氧体晶相结构和形貌的分析表明,循环过程中经过“还原-氧化”后生成的NiO和载氧体颗粒团聚是导致载氧体活性下降的主要原因。相较于载热作用,NiFeAlO4载氧体在煤化学链燃烧中主要起供氧作用,它不仅会促进挥发分向煤气的转化,而且NiFeAlO4载氧体与焦炭之间也存在固固反应,利于更多CO2气体的生成。

       

      Abstract: Fe-based oxygen carrier is regarded as a promising industrial oxygen carrier,but there are some problems of low oxygen utilization rate and easy sintering at high temperatures.Although the performance of Fe-based oxygen carriers can be improved by preparing bimetallic composite oxygen carriers or adding inert components,there are certain defects.If the active components and inert materials can be integrated into a crystal structure to prepare oxygen carrier with spinel structure,the synergistic effect of bimetal can be used to improve the activity performance of oxygen carrier while Al~(3+) is employed to improve the stability of oxygen carrier.The NiFeAlO_4 oxygen carrier with spinel structure were synthesized via co-precipitation method and sol-gel method.The effects of preparation method and mass ratio(oxygen carrier to coal) on the coal chemical looping combustion reaction and cycling stability of the NiFeAlO_4 oxygen carrier were experimentally investigated.The function of oxygen carrier in coal conversion was also studied.The results show that NiFeAlO_4 oxygen carrier synthesized by sol-gel method possesses superior reactivity.When the mass ratio between oxygen carrier and coal was 20∶1,the carbon conversion is 86.7%,which is higher than that of coal pyrolysis(34%),and the CO_2 relative concentration is 93.6%.The analysis of the crystal structure and morphology of NiFeAlO_4 oxygen carrier before and after the reaction shows that the Ni O detected after 10th redox cycle and the grain agglomeration are the main reason for the decrease of its cyclic stability.Compared to its heating supply function,NiFeAlO_4 oxygen carrier mainly plays the role of oxygen supply in coal chemical looping combustion,which not only promotes the conversion of volatile matter to coal gas,but also has solid-solid reaction between NiFeAlO_4 oxygen carrier and coke,and is conducive to the generation of more CO_2.

       

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