炭材料-Ni催化剂上焦炉气二氧化碳催化重整制合成气
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摘要
本文采用炭材料与Ni基金属材料作为催化剂对焦炉气二氧化碳重整制合成气进行了系统研究。深入考察了反应温度、空速、气氛等关键参数对重整反应的影响；并对催化剂稳定性和碳消耗特性进行了分析，进一步探讨了炭材料-Ni/Al2O3催化剂上CH4-CO2重整反应机理及动力学模型建立。结果表明，炭材料的存在有效缓解了Ni的烧结，降低催化剂表面积碳量和副产物水产率，使炭材料-Ni/Al2O3催化剂在重整反应中表现出显著的协同作用、较高的催化活性和稳定性；焦炉气中H2的存在导致逆水汽变换反应的发生，降低甲烷的转化率同时有利于CO2的转化，而CO的影响较小；重整反应稳定后的混合催化剂积碳-消碳行为类似于Ni/Al2O3催化剂，无明显的碳消耗；炭材料-Ni/Al2O3催化重整反应活化能更接近单一Ni/Al2O3催化剂，从动力学层面验证了其高效催化活性；为焦炉气二氧化碳重整用新型催化剂的制备提供科学指导和技术支撑。
This paper put forward the systematically study on the production of syngas from the reformingof carbon dioxide and coke oven gas using carbon material and Ni-based catalysts. The studyinvestigated the effect of some key parameters, such as reaction temperature, volumetric hourlyspace velocity（VHSV） and gas phenomenon, on the reforming reaction. Both the stability ofcatalysts and the properties of the carbon consumption were analyzed; Moreover, the mechanismand kinetics model of reforming of CH4-CO2with AC-Ni/Al2O3as catalyst were also established.The results show that carbon material has effectively effect on the reducing the sintering of Ni,carbon deposition on surface of catalysts and the yield of water, which can make AC-Ni/Al2O3hassignificant synergistic effect on the reforming reaction, higher catalytic activity and stability. H2incoke oven gas will lead to reverse water gas shift reaction, which will lower the conversion of CH4,and improve the conversion of CO2, but has little effect of CO. The action of carbon deposition andelimination of the blending catalyst over the stable reforming reaction is similar to single Ni/Al2O3,which has no significant carbon consumption. Then, over the mechanism and kinetics study, thehigh catalytic activity of carbon-Ni/Al2O3was proved in kinetics aspects. At last, it is expected thatthis study could provide some scientific guidance and technical support on production of syngasover reforming of coke oven gas and carbon dioxide.
This paper put forward the systematically study on the production of syngas from the reformingof carbon dioxide and coke oven gas using carbon material and Ni-based catalysts. The studyinvestigated the effect of some key parameters, such as reaction temperature, volumetric hourlyspace velocity（VHSV） and gas phenomenon, on the reforming reaction. Both the stability ofcatalysts and the properties of the carbon consumption were analyzed; Moreover, the mechanismand kinetics model of reforming of CH4-CO2with AC-Ni/Al2O3as catalyst were also established.The results show that carbon material has effectively effect on the reducing the sintering of Ni,carbon deposition on surface of catalysts and the yield of water, which can make AC-Ni/Al2O3hassignificant synergistic effect on the reforming reaction, higher catalytic activity and stability. H2incoke oven gas will lead to reverse water gas shift reaction, which will lower the conversion of CH4,and improve the conversion of CO2, but has little effect of CO. The action of carbon deposition andelimination of the blending catalyst over the stable reforming reaction is similar to single Ni/Al2O3,which has no significant carbon consumption. Then, over the mechanism and kinetics study, thehigh catalytic activity of carbon-Ni/Al2O3was proved in kinetics aspects. At last, it is expected thatthis study could provide some scientific guidance and technical support on production of syngasover reforming of coke oven gas and carbon dioxide.
引文
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