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Bi-reforming of methane on Ni/SBA-15 catalyst for syngas production: Influence of feed composition

机译:甲烷在Ni / SBA-15催化剂上重整甲烷以生产合成气:进料组成的影响

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Bi-reforming of methane (BRM) was evaluated for Ni catalyst dispersed on SBA-15 support prepared by hydrothermal technique. BRM reactions were conducted under atmospheric condition with varying reactant partial pressure in the range of 10-45 kPa and 1073 K in fixed-bed reactor. The ordered hexagonal mesoporous SBA-15 support possessing large specific surface area of 669.5 m(2) g(-1) was well preserved with NiO addition during incipient wetness impregnation. Additionally, NiO species with mean crystallite dimension of 14.5 nm were randomly distributed over SBA-15 support surface and inside its mesoporous channels. Thus, these particles were reduced at various temperatures depending on different degrees of metal-support interaction. At stoichiometric condition and 1073 K, CH4 and CO2 conversions were about 61.6% and 58.9%, respectively whilst H-2/CO ratio of 2.14 slightly superior to theoretical value for BRM would suggest the predominance of methane steam reforming. H-2 and CO yields were significantly enhanced with increasing CO2/(CH4 + H2O) ratio due to growing CO2 gasification rate of partially dehydrogenated species from CH4 decomposition. Additionally, a considerable decline of H-2 to CO ratio from 2.14 to 1.83 was detected with reducing H2O/(CH4 + CO2) ratio due to dominant reverse water-gas shift side reaction at H2O-deficient feedstock. Interestingly, 10%Ni/SBA-15 catalyst was resistant to graphitic carbon formation in the co-occurrence of H2O and CO2 oxidizing agents and the mesoporous catalyst structure was still maintained after BRM. A strong correlation between formation of carbonaceous species and catalytic activity was observed. (C) 2018 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:对于通过水热技术制备的SBA-15载体上分散的Ni催化剂,对甲烷(BRM)进行了双重整。在固定床反应器中,BRM反应在大气条件下进行,反应物分压在10-45 kPa和1073 K范围内变化。有序的六角形介孔SBA-15支撑物具有669.5 m(2)g(-1)的大比表面积,在初期湿润浸渍过程中通过添加NiO可以很好地保存。此外,平均晶粒尺寸为14.5 nm的NiO物种随机分布在SBA-15支撑表面及其中孔通道内部。因此,取决于金属-载体相互作用的不同程度,这些颗粒在各种温度下被还原。在化学计量条件下和1073 K,CH4和CO2的转化率分别约为61.6%和58.9%,而H-2 / CO比2.14略高于BRM的理论值,这表明甲烷蒸汽重整的优势。 H-2和CO产率随着CO2 /(CH4 + H2O)比的增加而显着提高,这是由于CH4分解引起的部分脱氢物种的CO2气化速率增加。另外,由于H2O /(CH4 + CO2)比的降低,由于在H2O缺乏的原料中占主导地位的反向水煤气变换副反应,H-2与CO的比值显着下降,从2.14降至1.83。有趣的是,在H2O和CO2氧化剂的共存下,10%Ni / SBA-15催化剂对石墨碳的形成有抵抗力,并且BRM后仍保持了介孔催化剂的结构。观察到碳质物质的形成与催化活性之间的强烈相关性。 (C)2018氢能出版物有限公司。由Elsevier Ltd.出版。保留所有权利。

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