{"title":"在水冷式 DBD 等离子体中通过甲烷部分氧化实现二氧化碳的价值化","authors":"Nicola Lisi, Umberto Pasqual Laverdura","doi":"10.1016/j.jcou.2024.102931","DOIUrl":null,"url":null,"abstract":"<div><div>The valorisation of carbon dioxide in chemical plasmas implies as a principal reaction step its energy efficient dissociation into carbon monoxide. For hydrogen production, the reaction carbon monoxide with water (WGS) may lead to the generation of green hydrogen and reusable carbon dioxide. Beyond hydrogen, most valorisation processes require the removal of O<sub>2</sub> to avoid its recombination with CO on any downstream hot catalytic surface. Moreover, if the oxygen scavenging is performed directly inside the plasma volume, it can also shift the dissociation equilibrium that is responsible for the well-known trade-off between energy efficiency and conversion, thus improving efficiency when larger specific energy densities are applied. In this paper we first report on the plasma dissociation of pure CO<sub>2</sub> in a water cooled, high power(<2 kW), Dielectric Barrier Discharge with high gas flow regime (<3600sccm), and then we explore the synergistic oxygen removal by the partial oxidation of methane for syngas production. 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引用次数: 0
摘要
化学等离子体中二氧化碳的价值化意味着其主要反应步骤是高效节能地解离成一氧化碳。在制氢方面,一氧化碳与水的反应(WGS)可生成绿色氢气和可重复使用的二氧化碳。除氢气外,大多数价化过程都需要去除氧气,以避免其在下游热催化表面与一氧化碳重新结合。此外,如果直接在等离子体内部进行氧气清除,还可以改变解离平衡,而解离平衡正是众所周知的能效与转化率之间权衡的结果,因此在应用较大的比能量密度时,可以提高效率。在本文中,我们首先报告了在水冷、高功率(2 kW)、高气体流量(3600sccm)的介质势垒放电条件下等离子体解离纯 CO2 的情况,然后我们探讨了通过部分氧化甲烷协同脱氧来生产合成气的问题。质量和光学发射光谱证实,即使是少量的 CH4,也能去除外流和排放区域的氧气,并从两个方面增强了工艺:它允许向系统输入 CH4 与 CO2 比率较低(0.1-0.3)的气体,而不是纯 CO2。3),而不是纯 CO2,因为垃圾填埋气和废气是不希望改变气候的排放物,其成分类似,目前需要燃烧;它还允许将反应器外流直接用于 WGS 反应器或任何其他 CO 值化工艺,而无需去除下游的 O2。
Carbon dioxide valorisation with partial oxidation of methane in a water cooled DBD plasma
The valorisation of carbon dioxide in chemical plasmas implies as a principal reaction step its energy efficient dissociation into carbon monoxide. For hydrogen production, the reaction carbon monoxide with water (WGS) may lead to the generation of green hydrogen and reusable carbon dioxide. Beyond hydrogen, most valorisation processes require the removal of O2 to avoid its recombination with CO on any downstream hot catalytic surface. Moreover, if the oxygen scavenging is performed directly inside the plasma volume, it can also shift the dissociation equilibrium that is responsible for the well-known trade-off between energy efficiency and conversion, thus improving efficiency when larger specific energy densities are applied. In this paper we first report on the plasma dissociation of pure CO2 in a water cooled, high power(<2 kW), Dielectric Barrier Discharge with high gas flow regime (<3600sccm), and then we explore the synergistic oxygen removal by the partial oxidation of methane for syngas production. The presence of CH4, even in small amounts, removes oxygen from the outstream and from the discharge region, as confirmed by mass and optical emission spectroscopies, and enhances the process in two ways: it allows to feed the system with gas having a low CH4 to CO2 ratio (0.1–0.3) instead of pure CO2, where landfill and waste gases are undesired climate altering emissions with a similar composition that currently require flaring; it will allow to use directly the reactor outstream into a WGS reactor, or any other CO valorisation process without the necessity to remove downstream O2.
期刊介绍:
The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials.
The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications.
The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.