本文關(guān)鍵詞：甲烷二氧化碳重整反應(yīng)鎳基和鈷基催化劑的制備及性能研究　出處：《內(nèi)蒙古大學(xué)》2015年碩士論文　論文類型：學(xué)位論文

  更多相關(guān)文章： CH_4/CO_2重整 鎳基 鈷基 載體 助劑 積炭

【摘要】：甲烷二氧化碳重整反應(yīng)可以有效地利用天然氣和消除溫室氣體,對解決能源危機和改善氣候環(huán)境問題具有廣闊的應(yīng)用前景而受到廣泛關(guān)注。本文針對CH4/CO2重整反應(yīng)催化體系,系統(tǒng)考察了活性組分、載體、助劑對催化性能的影響。本文采用初濕浸漬法制備了兩種體系的CH4/CO2重整反應(yīng)催化劑,通過XRD、N2吸附-脫附、化學(xué)吸附(H2-02滴定、H2-TPR)、SEM、TEM-EDAX、 TG-DTA等表征手段,分析了催化劑的物相組成、織構(gòu)性質(zhì)、金屬分散度、還原性、形貌以及積炭等,考察了催化劑前驅(qū)體、活性組分負(fù)載量、載體對CH4/CO2重整反應(yīng)活性及穩(wěn)定性的影響,分別探究了同一載體不同活性組分對催化性能的影響。以介孔氧化鋁為載體,制備了系列鎳基催化劑x%Ni/OMA (x=5、0、15、20)和鈷基催化劑x%Co/OMA (x=5、10、15、20),結(jié)果表明：金屬分散度受活性金屬負(fù)載量的影響,OMA表現(xiàn)出較強的金屬-載體相互作用；常壓、800℃C、空速為6000ml/g/h條件下反應(yīng)20h,10%Ni/OMA的轉(zhuǎn)化率和選擇性均沒有明顯的下降,CH4和C02的轉(zhuǎn)化率保持在98%、85%,H2/CO接近于1,催化活性較好。15%Co/OMA CH4和CO2的轉(zhuǎn)化率分別在95%、35%,H2/CO接近1.2,積炭少催化活性較好,整體來看,10%Ni/OMA催化活性要高于15%Co/OMA。因為OMA顯酸性,利于甲烷的吸附和活化,但不易于CO2的吸附和轉(zhuǎn)化,于是采用Y2O3作為載體助劑,合成了介孔釔鋁氧復(fù)合氧化物(YAG),以YAG為載體,制備了系列鎳基x%Ni/YAG (x=5、10、15、20)和鈷基催化劑x%Co/YAG (x=5.10、15、20)用于甲烷二氧化碳重整反應(yīng),研究發(fā)現(xiàn)：稀土釔的加入,提高了催化劑的金屬分散度,降低活性組分的還原溫度,增強催化劑的抗積炭性能,確定最佳反應(yīng)溫度為800℃。系列鎳基催化劑中20%Ni/YAG積炭少,CH4、 CO2轉(zhuǎn)化率分別達到95%、60%而積炭量較少,催化活性較好。15%Co/YAG的CH4、CO2轉(zhuǎn)化率分別達到95%、60%而積炭量較少。相同反應(yīng)條件下,20%Ni/YAG催化劑的催化性能好于15%Co/YAG。
[Abstract]:The carbon dioxide reforming of methane can effectively utilize the natural gas and the elimination of greenhouse gases, is to solve the problem of energy crisis and improve the climate and environment the broad application prospect and attracted widespread attention. In this paper CH4/CO2 catalytic reforming reaction system, investigated the active component and carrier, effect of additives on the catalytic performance. This paper uses the wet impregnation method preparation of two kinds of CH4/CO2 reforming catalyst by XRD, N2 adsorption desorption, chemical adsorption (H2-02 titration, H2-TPR, SEM, TEM-EDAX, TG-DTA) by means of analysis of the phase composition of the catalyst material texture properties, metal dispersion, reducibility, morphology and deposition, were investigated the precursor of the catalyst, the active component loading, carrier reaction activity and stability of CH4/CO2 reforming, respectively on the same carrier effect of different active component on the catalytic performance of mesoporous oxygen. Aluminum as the carrier, series of nickel based catalysts were prepared by x%Ni/OMA (x=5,0,15,20) and cobalt based catalyst x%Co/OMA (x=5,10,15,20), the results show that the metal dispersion affected by active metal loading, OMA showed strong metal support interaction; atmospheric pressure, 800 degrees C, space velocity of 6000ml/g/h reaction under the conditions of 20h. The conversion of 10%Ni/OMA and selectivity are not significantly reduced, CH4 and C02 conversion rate remained at 98%, 85%, H2/CO is close to 1, conversion of better catalytic activity and CO2.15%Co/OMA CH4 respectively in 95%, 35%, H2/CO is close to 1.2, the carbon deposit less good catalytic activity, overall, the photocatalytic activity is higher than 10%Ni/OMA 15%Co/OMA. because OMA is acidic, conducive to methane adsorption and activation, but not easy to adsorption and transformation of CO2, and using Y2O3 as carrier additives, mesoporous alumina synthesized yttrium oxides (YAG), with YAG as the carrier, the preparation of nickel series Based x%Ni/YAG (x=5,10,15,20) and x%Co/YAG (x=5.10,15,20) cobalt based catalyst for carbon dioxide reforming of methane reaction, the results showed that adding yttrium, improves the catalyst metal dispersion, reduce the reduction temperature of the active components, enhanced resistance to carbon deposition of the catalyst, the optimum reaction temperature is 800 DEG C. 20%Ni/YAG series of nickel based catalyst in less carbon deposition, CH4, CO2 conversion rate reached 95% and 60% respectively, the coke quantity is less, better catalytic activity of.15%Co/YAG CH4, CO2 conversion rate reached 95% and 60% respectively, the amount of coke deposited less. Under the same reaction conditions, the catalytic performance of 20%Ni/YAG catalyst was better than 15%Co/YAG.

【學(xué)位授予單位】：內(nèi)蒙古大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TE665.3;O643.36

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本文編號：1405434