Nitrogen Fixation by Gliding Arc Plasma: Better Insight by Chemical Kinetics Modelling.
Nitrogen Fixation by Gliding Arc Plasma: Better Insight by Chemical Kinetics Modelling.
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DOI：
10.1002/cssc.201700095
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发表时间：
2017-05
期刊：
影响因子：
8.4
通讯作者：
Weizong Wang;B. Patil;S. Heijkers;V. Hessel;A. Bogaerts
中科院分区：
文献类型：
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作者：
Weizong Wang;B. Patil;S. Heijkers;V. Hessel;A. Bogaerts
由于在生物圈氮循环中的重要作用，将大气中的氮转化为有价值的化合物，即所谓的固氮作用，正日益引起人们的兴趣。等离子体技术，更具体地说，滑动弧等离子体，在这一领域有很大的潜力，但鲜为人知的基本机制。因此，我们开发了一个详细的化学动力学模型的脉冲功率滑弧反应器在大气压下操作的氮氧化物合成。实验进行验证模型和合理的协议之间的计算和测量的NO和NO2产量和相应的能量效率为NOx形成不同的N2 /O2比，表明该模型可以提供一个现实的等离子体化学的图片。因此，我们可以使用该模型来研究NOx的形成和损失的反应途径。结果表明，振动激发的N2在滑动电弧中的显着贡献，以激活N2分子，并导致一个能量有效的方式产生的NOx，相比，热过程。基于基础化学，该模型使我们能够提出如何通过滑动电弧技术进一步改善NOx形成的解决方案。虽然目前阶段基于滑动弧的固氮工艺的能源效率无法与世界规模的哈伯-博世工艺相比，但我们相信我们的研究有助于我们提出更现实的方案，在农业肥料分散生产的新商业案例中进入尖端创新，其中低温等离子体技术可能发挥重要作用。
The conversion of atmospheric nitrogen into valuable compounds, that is, so-called nitrogen fixation, is gaining increased interest, owing to the essential role in the nitrogen cycle of the biosphere. Plasma technology, and more specifically gliding arc plasma, has great potential in this area, but little is known about the underlying mechanisms. Therefore, we developed a detailed chemical kinetics model for a pulsed-power gliding-arc reactor operating at atmospheric pressure for nitrogen oxide synthesis. Experiments are performed to validate the model and reasonable agreement is reached between the calculated and measured NO and NO2 yields and the corresponding energy efficiency for NOx formation for different N2 /O2 ratios, indicating that the model can provide a realistic picture of the plasma chemistry. Therefore, we can use the model to investigate the reaction pathways for the formation and loss of NOx . The results indicate that vibrational excitation of N2 in the gliding arc contributes significantly to activating the N2 molecules, and leads to an energy efficient way of NOx production, compared to the thermal process. Based on the underlying chemistry, the model allows us to propose solutions on how to further improve the NOx formation by gliding arc technology. Although the energy efficiency of the gliding-arc-based nitrogen fixation process at the present stage is not comparable to the world-scale Haber-Bosch process, we believe our study helps us to come up with more realistic scenarios of entering a cutting-edge innovation in new business cases for the decentralised production of fertilisers for agriculture, in which low-temperature plasma technology might play an important role.