微流动反应器中甲烷热解与氢气生成的压力和温度依赖性
Pressure and temperature dependence of methane pyrolysis and hydrogen production in a micro flow reactor
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中文总结 AI 辅助
本研究在微流动反应器中实验研究了甲烷热解制氢，发现模拟在高温下能复现压力趋势，但低温下需改进PAH动力学以提高预测能力。
中文摘要 AI 辅助
在微流动反应器中进行了甲烷热解实验，以研究在升高的压力和温度下化学机制的敏感性。本研究中使用的微流动反应器能够独立控制反应参数。实验在1400至1800 K的温度范围和1至10 bar的压力范围内进行，固定停留时间为60 ms。定量测定了氢气、未反应甲烷和固体碳的产率，以便与预测模型进行比较。同时定量了非均相沉积物的质量。通过气相色谱-质谱联用（GC-MS）测量了C2和多环芳烃（PAH）物种的存在。实验结果与使用离散分段模型的一维模拟进行了比较，该模型用于捕捉颗粒形成和表面沉积的动力学。模拟在高温（1800 K）下很好地再现了压力趋势，但对温度的敏感性与实验不一致。模拟通常发现碳和氢的产率低于实验值，且对温度的敏感性更强。在较低温度和较高压力下测量到了大量的PAH中间体。模拟的表面沉积速率低于测量值，但显示出相似的分布特征。结果表明，微流动反应器在模拟甲烷制氢的热解环境方面具有实用性。通过改进低温下燃料分解以及PAH形成和消耗动力学，并对表面位点密度进行详细处理，可以提高模拟的预测能力。
英文摘要
Methane pyrolysis experiments were performed in a micro flow reactor to investigate the chemical mechanism sensitivities at elevated pressures and temperatures. The micro flow reactor used in this study provides independent control over reaction parameters. Experiments were performed at temperatures from 1400 to 1800 K and pressures from 1 to 10 bar at a fixed residence time of 60 ms. The yields of hydrogen, unreacted methane, and solid carbon were quantified for comparison to predictive models. The mass of heterogeneous depositions was also quantified. The presence of C2 and PAH species were measured by GC-MS. The results were compared to 1D simulations using a discrete sectional model for capturing the kinetics of particulate formation and surface deposition. The simulations replicated the pressure trend well at high temperatures (1800 K), but the sensitivity to temperature was in disagreement. Simulations generally found lower carbon and hydrogen yields and a stronger sensitivity to temperature than the experiment. An abundance of PAH intermediates was measured at lower temperatures and higher pressures. The simulated surface deposition rates were lower than the measured values but showed similar profiles. The results demonstrate the utility of micro flow reactors in recreating pyrolysis environments for hydrogen production from methane. The predictive capabilities of simulations could be improved by advancing the fuel decomposition and PAH formation and consumption kinetics at low temperatures and by detailed treatment of surface site density.
发表机构
- University of Toronto Institute for Aerospace Studies（多伦多大学航空航天研究所）
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