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评估不同介电阻挡放电等离子体构型作为替代技术,用于二氧化碳重整甲烷和甲醇直接分解中的绿色 C1 化学。

Evaluation of different dielectric barrier discharge plasma configurations as an alternative technology for green C1 chemistry in the carbon dioxide reforming of methane and the direct decomposition of methanol.

机构信息

Instituto de Ciencia de Materiales de Sevilla (CSIC-Universidad de Sevilla), Spain.

出版信息

J Phys Chem A. 2010 Mar 25;114(11):4009-16. doi: 10.1021/jp100346q.

DOI:10.1021/jp100346q
PMID:20184329
Abstract

Carbon dioxide reforming of methane and direct decomposition of methanol have been investigated using dielectric barrier discharges (DBD) at atmospheric pressure and reduced working temperatures. Two different plasma reactor configurations are compared and special attention is paid to the influence of the surface roughness of the electrodes on the conversion yields in the first plasma device. The influence of different filling gap dielectric materials (i.e., Al(2)O(3) or BaTiO(3)) in the second packed configuration has been also evaluated. Depending on the experimental conditions of applied voltage, residence time of reactants, feed ratios, or reactor configuration, different conversion yields are achieved ranging from 20 to 80% in the case of methane and 7-45% for the carbon dioxide. The direct decomposition of methanol reaches 60-100% under similar experimental conditions. Interestingly, the selectivity toward the production of hydrogen and carbon monoxide is kept almost constant under all the experimental conditions, and the formation of longer hydrocarbon chains or coke as a byproduct is not detected. The maximum efficiency yields are observed for the packed-bed reactor configuration containing alumina for both reaction processes (approximately 1 mol H(2) per kilowatt hour for dry reforming of methane and approximately 4.5 mol H(2) per kilowatt hour for direct decomposition of methanol).

摘要

在大气压和降低的工作温度下,使用介质阻挡放电(DBD)研究了甲烷的二氧化碳重整和甲醇的直接分解。比较了两种不同的等离子体反应器构型,并特别关注了第一台等离子体设备中电极表面粗糙度对转化率的影响。还评估了在第二种填充间隙介电材料(即 Al2O3 或 BaTiO3)的第二填充构型中不同的影响。根据施加电压、反应物停留时间、进料比或反应器构型的实验条件,不同的转化率可达到 20-80%甲烷和 7-45%二氧化碳的范围。在类似的实验条件下,甲醇的直接分解达到 60-100%。有趣的是,在所有实验条件下,生产氢气和一氧化碳的选择性几乎保持不变,并且没有检测到较长的碳氢链或焦炭作为副产物的形成。对于包含氧化铝的填充床反应器构型,两种反应过程的最大效率产率都被观察到(甲烷干重整时每千瓦小时约 1 摩尔 H2,甲醇直接分解时每千瓦小时约 4.5 摩尔 H2)。

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