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Thermodynamic and Kinetic Study of Carbon Dioxide and Mercury Removal from Flue Gas in Coal Combustion Power Plants.

机译:燃煤电厂烟气中二氧化碳和汞去除的热力学和动力学研究。

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摘要

Carbon dioxide and mercury from anthropogenic emissions pose a significant threat to our environment and human health. Removal from their major source - coal-fired power plants - is one of the most effective approaches to control their emissions. Thermodynamics and kinetics are critical to the studies of the removal technologies as they provide fundamental knowledge of the capture process. In this work, the thermodynamics and kinetics of CO2 and Hg capture through absorption using aqueous amines solutions and adsorption using supported ionic liquid sorbents were investigated.;A vapor-liquid equilibrium (VLE) data reduction method that simplifies experimental measurements while maintaining accuracy was applied for the first time to the thermodynamic study of CO2 absorption in aqueous amine systems. The method eliminates the measurements of speciation in liquid phase and vapor phase by applying a layer of mass balance iteration in the correlation. Incorporating the electrolyte non-random two liquid (eNRTL) model and the Soave-Redlich-Kwong (SRK) model, the data reduction method was used to correlate VLE and heat of absorption data collected in a modified batch calorimeter for ethanolamine (MEA) - H2O - CO2 system and piperazine (PZ) - H2O - CO2 systems. The optimized model with the best-fit eNRTL model parameters was used to predict vapor pressures under the conditions reported in the literature; the predicted values were consistent with the independent literature results, indicating successful application of the Barker data reduction method and the mathematical model in the thermodynamic study of CO2-aqueous amine systems.;With the current technologies, capture of CO2 and Hg from coal combustion flue gas requires additional air pollution control devices that can only do a single task. To reduce the cost, a new approach to capture both CO2 and Hg from coal combustion flue gas in an integrated adsorbent system was discovered. In this approach, a task-specific amino acid ionic liquid is supported on silica gel particles with high surface area and pore volume. The CO2 capacity for was found to be 0.4 mol of CO 2/ mol of ionic liquid. The ionic liquid loading was optimal for CO 2 capture at 40 wt%. Mass transfer in fixed-bed trials was slow at high ionic liquid loadings due to the decreasing in contact surface area. Hg capture performance was assessed for the same material under a nitrogen environment. These sorbent systems had a total Hg uptake of more than 14 mg/g. Slipstream testing of the sorbents, along with other novel Hg sorbents developed previously, using coal combustion flue gas showed promising and competitive results in Hg removal rate and Hg capacity. When both CO2 and Hg are present in the gas phase, it is expected that Hg accumulates and fixes in the sorbent via strong chemical bonding over an extended time, while CO2 can reversibly be adsorbed and desorbed on the sorbent. This hypothesis was validated by the experimental evidence that the present of CO2 has limited effect on the capture of elemental Hg vapor and the theoretical evidence that oxidized Hg has a stronger bonding with the ionic liquid than CO2.
机译:人为排放产生的二氧化碳和汞对我们的环境和人类健康构成重大威胁。从主要排放源(燃煤电厂)中清除是控制其排放的最有效方法之一。热力学和动力学对去除技术的研究至关重要,因为它们提供了捕获过程的基础知识。在这项工作中,研究了通过胺水溶液的吸收和负载型离子液体吸附剂的吸附而捕获CO2和Hg的热力学和动力学。汽-液平衡(VLE)数据减少方法可简化实验测量并同时保持精度首次用于胺水溶液中CO2吸收的热力学研究。通过在相关中应用质量平衡迭代层,该方法消除了液相和气相中形态分析的测量。结合电解质非随机两液(eNRTL)模型和Soave-Redlich-Kwong(SRK)模型,数据缩减方法用于将VLE与在乙醇胺(MEA)的改进的分批热量计中收集的吸收数据的热量相关联- H2O-CO2系统和哌嗪(PZ)-H2O-CO2系统。具有最佳拟合eNRTL模型参数的优化模型可用于预测文献报道条件下的蒸气压。预测值与独立文献结果吻合,表明Barker数据还原方法和数学模型在CO2-水胺系统热力学研究中的成功应用。;利用现有技术,从燃煤烟道中捕集CO2和Hg天然气需要额外的空气污染控制设备,这些设备只能完成一项任务。为了降低成本,人们发现了一种在集成吸附剂系统中从燃煤烟气中捕获二氧化碳和汞的新方法。在这种方法中,具有特定任务的氨基酸离子液体被支撑在具有高表面积和孔体积的硅胶颗粒上。发现其的CO 2容量为0.4摩尔CO 2 /摩尔离子液体。离子液体载量对于40 wt%的CO 2捕集是最佳的。在固定床试验中,由于接触表面积的减少,在高离子液体载量下传质很慢。在氮气环境下,对相同材料的汞捕获性能进行了评估。这些吸附剂系统的总汞吸收量超过14 mg / g。使用煤燃烧烟道气对吸附剂以及其他以前开发的其他新型汞吸附剂进行滑流测试,结果表明,在汞去除率和汞容量方面,前景看好且具有竞争力。当气相中同时存在CO2和Hg时,预计Hg会在很长一段时间内通过牢固的化学键在吸附剂中积聚并固定,而CO2可以可逆地吸附和脱附在吸附剂上。这一假设已得到以下实验证据的证实:存在的CO2对元素汞蒸气的捕集具有有限的影响,以及被氧化的Hg与离子液体的结合力比CO2强的理论证据。

著录项

  • 作者

    Liu, Kun.;

  • 作者单位

    University of Cincinnati.;

  • 授予单位 University of Cincinnati.;
  • 学科 Engineering Chemical.
  • 学位 Ph.D.
  • 年度 2012
  • 页码 251 p.
  • 总页数 251
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

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