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Development of tailor-made oxygen carriers and reactors for chemical looping processes at Huazhong University of Science & Technology
International Journal of Greenhouse Gas Control ( IF 4.6 ) Pub Date : 2019-11-22 00:00:00 , DOI: 10.1016/j.ijggc.2019.102898
Haibo Zhao , Xin Tian , Jinchen Ma , Mingze Su , Baowen Wang , Daofeng Mei

For the concerns of global warming, there is an urgent need of green, low-cost, and sustainable ways for the conversion and utilization of fossil energy. Holding the merit of inherent CO2 separation during carbonaceous fuel conversion, chemical looping technique is emerging as a perfect alternative to conventional fossil fuel conversion processes. Central to this technique is the design of high-performance oxygen carriers and suitable reactors that can efficiently realize the cyclic redox loop involved. To date, plenty kinds of (over 1200) oxygen carriers have been screened, synthesized and investigated by different research groups worldwide. Dozens of chemical looping reactors with thermal power ranged from kWth to MWth were also constructed and successfully operated. All these help to support the commercial demonstration and even industrial application of this innovative fuel conversion and carbon capture technique.

The chemical looping related research at Huazhong University of Science & Technology (HUST) has experienced rapid development during the past 10 years, from rational synthesis of oxygen carrier to inter-connected fluidized bed reactor design and operation. In this article, the development of tailor-made oxygen carriers and active design of reactors at HUST is comprehensively reviewed and appraised, including the screening and optimization of oxygen carriers, reduction kinetics of oxygen carriers with gaseous fuels, microcosmic level understanding of the reaction mechanism in chemical looping via density functional theory (DFT) calculation, rational design and controllable synthesis of a hierarchically-structured oxygen carrier, and negative effects of pollutants (like sulfur and chlorides) on oxygen carriers. Moreover, experience gained from the design, macro simulation and modeling as well as continuous operation of inter-connected fluidized bed reactors is also provided. Overall, more than 100 different oxygen carriers based on Fe-, Cu-, Mn-, Ni-, as well as mixed oxides and natural ores, are systematically reviewed in terms of different chemical looping processes. The rational design route of a representative CuO@TiO2-Al2O3 oxygen carrier is proposed from the bottom up, on the basis of DFT calculation, molecular dynamic (MD) simulation, and detailed kinetics analysis. Over 300 h of continuous operation experience of the inter-connected fluidized bed reactor contributes to the demonstration of this technique. Numerical simulation via commercial computational fluid dynamics (CFD) software further helped the design, optimization, and scale-up of the reactor. In general, this review paper outlines the research route of chemical looping at HUST in details, which is expected to provide useful reference and guidance for the relevant readers.



中文翻译:

华中科技大学开发用于化学循环过程的量身定制的氧气载体和反应器

对于全球变暖的关注,迫切需要绿色,低成本和可持续的方式来转化和利用化石能源。由于具有在含碳燃料转化过程中固有的CO 2分离优点,因此,化学循环技术正在成为传统化石燃料转化工艺的完美替代方案。该技术的核心是高性能氧气载体和合适的反应器的设计,这些反应器可以有效地实现所涉及的循环氧化还原回路。迄今为止,全球不同的研究小组已经筛选,合成和研究了多种(超过1200种)氧气载体。热功率从kW th到MW th的数十个化学回路反应器也被建造并成功运行。所有这些都有助于支持这种创新的燃料转化和碳捕集技术的商业示范甚至工业应用。

从合理合成氧气载体到互连流化床反应器的设计和运行,华中科技大学(HUST)的化学循环相关研究在过去十年中经历了飞速发展。在本文中,对HUST量身定制的氧气载体的开发和反应器的主动设计进行了全面的评估和评估,包括氧气载体的筛选和优化,用气体燃料还原氧气载体的动力学,对反应机理的微观层面的了解通过化学循环密度泛函理论(DFT)的计算,合理设计和可控制的分层结构氧载体的合成,以及污染物(如硫和氯化物)对氧载体的负面影响。此外,还提供了从相互连接的流化床反应器的设计,宏观仿真和建模以及连续操作中获得的经验。总体而言,根据不同的化学循环过程,系统地审查了基于铁,铜,锰,镍,混合氧化物和天然矿石的100多种不同的氧载体。代表性的CuO @ TiO 2 -Al 2 O 3的合理设计路线在DFT计算,分子动力学(MD)模拟和详细的动力学分析的基础上,自下而上地提出了氧载体。相互连接的流化床反应器超过300小时的连续运行经验为该技术的示范做出了贡献。通过商业计算流体动力学(CFD)软件进行的数值模拟进一步帮助了反应器的设计,优化和放大。总的来说,这篇综述文章详细概述了科大化学环的研究路线,有望为相关读者提供有用的参考和指导。

更新日期:2019-11-22
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