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Plasmachemical Synthesis of Carbon Suboxide

机译:等离子体化学合成二氧化碳

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摘要

A nonthermal carbon monoxide plasma is known to produce a solid deposition which is thought to be a polymer of carbon suboxide (C3O2); however there are very few investigations of this deposition in the literature. This thesis contains an analysis of the theoretical thermodynamics and kinetics of carbon suboxide formation as well as experimental results. The theoretical analysis suggests that carbon suboxide may be an equilibrium product even at ambient conditions but favors lower temperatures; furthermore if solid carbon is considered to be kinetically limited, and therefore not a product, then carbon suboxide is more likely to be a product under these pseudo-equilibrium conditions. Experimentally, solid films were produced in a dielectric barrier discharge (DBD) containing pure carbon monoxide. Optical emission spectroscopy was used to analyze the plasma and models of the emission spectra were created to determine the plasma temperatures. Deposition rates were determined to be on the order of 0.2 mg/min at a power of about 10W; it is expected however that these conditions are not optimized. The overall kinetics of carbon suboxide was analyzed and optimal conditions for operation can be estimated. Characterization of the solid depositions were carried out using Solid State Nuclear Magnetic Resonance (NMR), Fourier Transform Infrared Spectroscopy (FTIR), Electrospray Ionization Mass Spectroscopy (ESI-MS), and Matrix-assisted Laser Desorption Ionization Mass Spectroscopy (MALDI-MS). The characteristics of the film are very comparable to hydrolyzed carbon suboxide polymer suggesting that carbon suboxide polymer were in fact created in the carbon monoxide plasma at atmospheric conditions.
机译:已知非热一氧化碳等离子体会产生固体沉积物,该沉积物被认为是低碳碳(C3O2)的聚合物。但是,文献中对此沉积的研究很少。本文对低碳氧化物形成的理论热力学和动力学以及实验结果进行了分析。理论分析表明,即使在环境条件下,二氧化碳也可能是平衡产物,但有利于降低温度。此外,如果认为固体碳在动力学上受限制,因此不是产物,那么在这些拟平衡条件下,次氧化碳更有可能是产物。实验上,在包含纯一氧化碳的介电势垒放电(DBD)中生产了固态膜。使用发射光谱法分析等离子体,并创建发射光谱模型以确定等离子体温度。在约10W的功率下,沉积速率确定为0.2 mg / min。但是,预计这些条件不会得到优化。分析了二氧化碳的整体动力学,可以估算出最佳操作条件。使用固态核磁共振(NMR),傅立叶变换红外光谱(FTIR),电喷雾电离质谱(ESI-MS)和基质辅助激光解吸电离质谱(MALDI-MS)对固体沉积物进行表征。该膜的特性与水解的一氧化碳聚合物非常相似,表明实际上在大气条件下在一氧化碳等离子体中产生了一氧化碳聚合物。

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    Geiger Robert;

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  • 年度 2013
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