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Methane decomposition kinetics and reaction rate over Ni/SiO2 nanocatalyst produced through co-precipitation cum modified Stober method

机译:共沉淀-改进斯托伯法制备Ni / SiO2纳米催化剂上甲烷的分解动力学和反应速率

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Co-precipitation cum modified Stober method was adopted to produce nano-Ni/SiO2 (n-Ni/SiO2) catalyst and conducted a series of methane decomposition kinetic experiments in a fixed bed pilot plant. Methane decomposition activity of n-Ni/SiO2 catalyst was quantified by considering thermodynamic deposition of carbon at a temperature range of 550-650 degrees C and methane partial pressure from 0.2 to 0.8 atm. The utmost methane conversion of 18.87 mmol/gcat min was obtained at 650 degrees C and methane partial pressure of 0.8 atm. The findings concluded that the enhancement occurred with carbon formation rate when increasing the methane partial pressure is very much evident at higher temperature such as 650 degrees C. However, the intensity in methane decomposition descending tendency was declined at lower reaction temperature. The effects of methane partial pressure and reaction temperature on the specific molar carbon formation rate were also examined. The calculated reaction order and activation energy were 1.40 and 61.1 kJ mol(-1), respectively. The kinetic experiments showed the existence of an optimum reaction condition to achieve the highest performance of n-Ni/SiO2 catalyst in terms of methane decomposition rate. However, carbon accumulation ceases once complete catalyst deactivation occurred at certain reaction conditions such as high temperature and lower methane partial pressure. Virgin nanocatalyst and as-produced nanocarbons were studied with BET, XRD, and TEM. 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
机译:采用共沉淀-改良斯托伯法制备纳米Ni / SiO2(n-Ni / SiO2)催化剂,并在固定床中试装置中进行了一系列甲烷分解动力学实验。 n-Ni / SiO2催化剂的甲烷分解活性通过考虑碳在550-650摄氏度的温度范围内的热力学沉积以及甲烷分压在0.2至0.8 atm的范围内进行定量。在650℃和0.8 atm的甲烷分压下,最高甲烷转化率为18.87 mmol / gcat min。该发现得出结论,在较高的温度例如650℃下,当增加甲烷分压时,随着碳形成速率的增加是非常明显的。然而,在较低的反应温度下,甲烷分解下降趋势的强度下降。还研究了甲烷分压和反应温度对比摩尔碳形成速率的影响。计算的反应顺序和活化能分别为1.40和61.1 kJ mol(-1)。动力学实验表明,存在最佳的反应条件以实现甲烷分解速率最高的n-Ni / SiO2催化剂性能。但是,一旦在某些反应条件下(例如高温和较低的甲烷分压)发生完全的催化剂失活,碳的积累就会停止。使用BET,XRD和TEM研究了原生纳米催化剂和所产生的纳米碳。 2016氢能出版物有限责任公司。由Elsevier Ltd.出版。保留所有权利。

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