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Microwave enhanced gasification of carbon.

机译:微波增强了碳的气化。

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摘要

The gasification of carbonaceous material is a long standing industrial process which produces valuable feed stocks of H2 and CO gas (Syngas) that can be reacted further resulting in extended hydrocarbons for use in numerous areas of industry. The process of gasification is energy intensive, requiring temperatures >700 °C, which at the industrial scale requires large amounts of excess energy in order to achieve optimal reaction temperatures for ideal compositions and product yields. Conventional convective heating methods of current industrial processes thereby limits the overall efficiency of the gasification process even before the desired product is achieved.;Microwave radiation of dipolar or conducting materials is known to produce heat in a significantly different way than conventional heating. Microwaves can specifically heat materials which in turn heats microwave active material to a higher temperature than by conventional methods because less heat is lost to surroundings with limited loss of excess energy to the complete system. It is understood that microwave radiation also leads to enhanced rates of reaction, due to its ability to selectively heat materials and the mechanism by which it heats. An industrially relevant process such as carbon gasification is therefore an ideal candidate for investigation.;The disproportionation of CO2 over carbon (Boudouard reaction) as a fundamental reaction in carbon gasification provided a clean and clear starting point in which to study the effects of microwave heating. It was found that the use of microwave radiation to selectively heat the carbon resulted in a profound change in the fundamental thermodynamics of the reaction. From kinetic studies of the reaction under conditions of flowing CO2, it was found that the apparent activation energy decreased from conventional convective heating to the modified system under microwave irradiation. From measurement of the equilibrium constants as a function of temperature, the enthalpy of the reaction also dropped under microwave irradiation. The change in enthalpy affected the position of the equilibrium so that the temperature at which CO becomes the major product dropped significantly from the conventional thermal reaction to the microwave. The changes in the fundamental thermodynamics of the reaction are attributed to the enhanced reactivity of the CO2 with the steady-state concentration of electron--hole pairs that are present at the surface of the carbon as a result of the space-charge mechanism, which is understood to be heating the carbon.;Such a mechanism is unique to microwave-induced heating, and, given the effect it has on the thermodynamics of the Boudouard reaction, suggests that its use may yield large energy savings in driving the general class of gas--carbon reactions. To further elucidate the significant increase in efficiency, the carbon-steam process was also examined under microwave irradiation. From equilibrium measurements of the carbon-steam, as well as the various equilibria of comprising secondary reactions, it was observed that the same type of thermodynamic enhancement occurred for this more complicated system.
机译:碳质材料的气化是一个长期存在的工业过程,它产生宝贵的H2和CO气原料(合成气),这些原料可以进一步反应,从而产生扩展的碳氢化合物,可用于许多工业领域。气化过程是高能耗的,需要温度> 700°C,在工业规模上需要大量的过量能量,以实现理想的反应温度,以实现理想的成分和产品收率。因此,当前工业过程的常规对流加热方法甚至在获得所需产品之前就限制了气化过程的整体效率。已知偶极或传导材料的微波辐射以与常规加热明显不同的方式产生热量。微波可以专门加热材料,从而将微波活性材料加热到比传统方法更高的温度,因为更少的热量散发到周围环境中,而整个系统的多余能量损失却有限。可以理解的是,由于微波辐射选择性加热材料的能力及其加热机理,微波辐射还可以提高反应速率。因此,与工业相关的过程(例如碳气化)是进行研究的理想选择。; CO2在碳上的歧化(Boudouard反应)是碳气化的基本反应,为研究微波加热的影响提供了一个清晰明确的起点。 。发现使用微波辐射选择性地加热碳导致反应的基本热力学的深刻变化。通过在流动的CO2条件下反应的动力学研究,发现表观活化能从常规的对流加热到微波辐射下的改性体系降低。从平衡常数作为温度的函数的测量,反应的焓在微波辐射下也降低了。焓的变化影响了平衡的位置,因此从常规的热反应到微波,CO成为主要产物的温度显着下降。反应的基本热力学变化归因于由于空间电荷机制而使CO2随碳表面上存在的电子-空穴对的稳态浓度增强的反应性,这是由于这种机制是微波感应加热所特有的,并且鉴于其对Boudouard反应热力学的影响,表明该方法的使用可能会在驱动一般的碳纳米管中产生大量的能量节省。气碳反应为了进一步阐明效率的显着提高,还在微波辐射下检查了碳蒸汽过程。从碳蒸汽的平衡测量以及包括次级反应在内的各种平衡,可以看出,对于这种更复杂的系统,发生了相同类型的热力学增强。

著录项

  • 作者

    Hunt, Jacob T.;

  • 作者单位

    The Florida State University.;

  • 授予单位 The Florida State University.;
  • 学科 Inorganic chemistry.
  • 学位 Ph.D.
  • 年度 2014
  • 页码 98 p.
  • 总页数 98
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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