【作者】 程华艺；

【导师】 沈彬； 孙岳明；

【作者基本信息】 东南大学 ， 材料物理与化学， 2006， 硕士

【摘要】 在半个多世纪以来,石油化工已发展成为现代文明社会的支柱产业。但由于石油资源的长期开采,储量已日趋下降。近年来原油的价格逐年攀高也正是这一危险信号的显现。我国西部蕴含着大量的天然气有待开发,为我们提供了一条开发能源的新途径。本文概述了CO2重整甲烷制合成气催化剂的抗积炭性能的研究进展,介绍了催化剂的活性组分、载体的选择对催化剂的影响以及碱土金属、稀土金属和贵重金属对催化剂改性的相关研究状况,同时还介绍了制备方法的改性状况,尤其是溶胶-凝胶法制备纳米级催化剂。综述了国内外近十年来的有关方面的研究。在此基础上,并通过反应的机理的推测,作了有关催化剂设计方面的理论探讨,选择了以γ-Al2O3载体,活性组分为镍,再添加贵金属金来改性催化剂的性能,金的前驱体选择了Au(NH3)4(NO3)2,制备方法采用传统的浸渍法。本文的实验部分通过运用脉冲反应技术,对不同组分的催化剂进行活性评价,以及对Au的不同前驱物的催化剂进了考察。并通过二氧化碳重整甲烷的连续反应活性评价,进一步考察了添加Au后的催化活性情况。在实验中考察了不同组分的催化剂,其中Au含量为0.7%的催化剂的稳定性和抗积炭性能表现最好。在此基础上,并考察了不同的反应温度和空速对催化剂的活性的影响。本文催化剂表征部分通过采用H2-TPR、NH3-TPD、XRD、SEM和TEM等手段对催化剂进行了表征,进行了一些理论上的讨论。H2-TPR表征结果显示催化剂的活性组分的分散性对催化剂的抗积炭性能有很大的促进作用,NH3-TPD表征结果显示催化剂的表面酸性中心的下降有利于提高二氧化碳的消炭性能,XRD结果表明添加Au后组分之间的相互作用对提高催化剂的抗积炭性能有积极作用,通过扫描电镜(SEM)对催化剂的形貌的观察发现,Au的添加改善了镍在载体表面的分散性能,通过透射电镜(TEM)对积炭后的催化剂的表面观察发现,添加Au后的催化剂表面上的丝状形积炭对二氧化碳的消炭有利。更多还原

【Abstract】 The petroleum chemical industry becomes the pillar industry in our modern civilized society since half century. But owing to the mining of petroleum resource over a long period of time, the reserves have descended day by day. Recently the oil price is increasing year by year is the danger signal about the issue. There is plenty of the natural gas remaining to be open in our west country, and provides a new way that is utilized the sources of energy for us.A review is carried out in the article about studying the catalyst in recent year which is used for the reforming of methane with carbon dioxide. Active component and support of catalyst is introduced. Rare earth metals and noble metals as promoter for catalyst are summarized comprehensively. And the preparation with sol-gel for catalyst nanoparticles is paid attention greatly. Methane reforming under microwave irradiation is mentioned. According to the suspect ion of the reactive mechanism, a theory discussion about the catalyst design is made in this paper. On the base of the discussion the catalyst is selected as: the supporter isγ-Al2O3;the active component is nickel; the noble mental of Au is added to modify the catalytic performance; and preparation method is the impregnation.The active evaluation of the catalyst with different Ni content is carried by the pulse reaction technology. And the article has test the action of different precursor of Au. The active performance of the catalyst after adding Au is inspected by the methane reforming with carbon dioxide. According to the experiment result,the catalyst of 0.7% Au content has show the best performance with good stability and good resistance to carbon deposited. On the basis of those, the different reaction temperature and space velocity is inspected for the catalytic activity.The characterized experiment is carried by the way of H2-TPR, NH3-TPD, XRD and SEM etc. From the characterized experiment result, H2-TPR tell us the good resistance to deposited carbon owing to the scattered active component; NH3-TPD show that the superficial acid center of catalyst influences the adsorption ability to the carbon dioxide; and XRD show that the interaction of different component after adding Au is helpful to the resistance to carbon deposited; SEM for the inspection of the catalyst surface show that the addition of Au can improve the Ni dispersion, and TEM result show that the addition of Au can increase the effect of the resistance to the carbon deposition.更多还原