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Reducible oxide based oxygen carriers for chemical looping combustion and partial oxidation of methane.

机译:基于可还原氧化物的氧气载体,用于化学循环燃烧和甲烷的部分氧化。

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摘要

Chemical looping combustion (CLC) is a novel combustion technology that offers a highly efficient route towards clean combustion of fuel with inherent CO2 capture. In CLC, a fuel is combusted in reducer reactor in contact with an oxygen carrier (typically a metal oxide) and subsequently re-oxidized by air in oxidizer. Condensation of steam from reducer effluent results in high purity sequestration ready CO2 streams. Thus CLC results in a NOx-lean, flame-less oxyfuel combustion process eliminating the need for air separation. Splitting the combustion into two half processes provides a high degree of flexibility in CLC for process intensification, e.g. a wide range of oxygen carriers, fuels and oxidant gases can be used, albeit use of various fuels/oxidants have their own challenges.;Typically in CLC, a metal is supported on a high temperature stable matrix to provide the required thermal stability in harsh redox conditions. However these non-reducible supports do not contribute any oxygen in the combustion process or facilitate the reduction of supported metal. Therefore in the present work, we test the applicability of reducible oxides like ceria as supports in CLC. It was found that, compared to non-reducible supports, the redox properties of ceria strongly facilitate efficient utilization of metal oxides in the process, thus resulting in improved redox kinetics and higher carrier conversion. The broad applicability of the concept was tested with various transition metals typically used in CLC. Furthermore, the reactivity of carriers was enhanced by employing systematically engineered mixed-oxides of iron, nickel and/or manganese.;Beyond combustion, tailoring the metal phase and reactor operation was used for partial oxidation of methane to produce syngas -- a valuable feedstock in chemical industry. Utilization of the looping concept for partial oxidation results in a safe oxidation process eliminating the need for expensive air separation or noble metal catalysts. Steam, CO2 or mixtures of both can be used as oxidants for ultra-pure H2 or syngas generation and CO2 activation. Current work underscores the fact that reactor operation in chemical looping allows targeting clean combustion, partial oxidation or various reforming processes, but rational design of oxygen carriers makes these processes viable.
机译:化学循环燃烧(CLC)是一种新颖的燃烧技术,它提供了一种高效的途径,可实现具有固有CO2捕集功能的清洁燃烧燃料。在CLC中,燃料在还原器反应器中燃烧,与氧气载体(通常是金属氧化物)接触,然后在氧化剂中被空气重新氧化。来自还原剂流出物的蒸汽冷凝会导致高纯度的二氧化碳封存。因此,CLC导致了NOx稀薄,无焰的含氧燃料燃烧过程,从而无需进行空气分离。将燃烧分为两个半过程可在CLC中为过程增强提供高度的灵活性,例如尽管使用各种燃料/氧化剂有其自身的挑战,但仍可以使用各种氧气载体,燃料和氧化剂气体。;典型地,在CLC中,将金属负载在高温稳定的基体上,以提供苛刻的热稳定性氧化还原条件。但是,这些不可还原的载体在燃烧过程中不会产生任何氧气,也不会促进负载金属的还原。因此,在本工作中,我们测试了可还原氧化物(如二氧化铈)在CLC中作为载体的适用性。已经发现,与不可还原的载体相比,二氧化铈的氧化还原性质强烈促进了该方法中金属氧化物的有效利用,因此导致氧化还原动力学的改善和载流子转化率的提高。使用CLC中通常使用的各种过渡金属测试了该概念的广泛适用性。此外,通过系统设计的铁,镍和/或锰的混合氧化物提高了载体的反应性;除燃烧外,还通过调整金属相和反应器操作来部分氧化甲烷以生产合成气-一种有价值的原料在化学工业中。利用环行概念进行部分氧化可实现安全的氧化过程,从而无需昂贵的空气分离或贵金属催化剂。蒸汽,CO2或两者的混合物可用作超纯H2或合成气生成和CO2活化的氧化剂。当前的工作强调了这样的事实,即在化学回路中的反应器操作允许针对清洁燃烧,部分氧化或各种重整过程,但是合理设计氧气载体使这些过程可行。

著录项

  • 作者

    Bhavsar, Saurabh Kiran.;

  • 作者单位

    University of Pittsburgh.;

  • 授予单位 University of Pittsburgh.;
  • 学科 Chemical engineering.
  • 学位 Ph.D.
  • 年度 2014
  • 页码 201 p.
  • 总页数 201
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

  • 入库时间 2022-08-17 11:54:12

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