本文選題：甲烷重整 + 工藝條件　； 參考：《安徽理工大學(xué)》2015年碩士論文

【摘要】：針對目前我國較為突出的環(huán)境問題,大量使用煤炭和石油作為能量來源并不符合國情發(fā)展。因此清潔的甲烷能源被人們所關(guān)注,尤其甲烷二氧化碳重整在制備合成氣方面表現(xiàn)出良好的環(huán)境效益和經(jīng)濟效益,但催化劑積炭問題使得此技術(shù)無法實現(xiàn)大規(guī)模工業(yè)化,眾多科研工作者從提升催化劑的抗積炭性能研究方向入手,但目前仍處于實驗研究階段。 本實驗則考慮到甲烷部分氧化重整和甲烷水蒸氣重整的優(yōu)勢有助于改善甲烷二氧化碳重整反應(yīng)性能,因此將甲烷二氧化碳重整、甲烷二氧化碳臨氧重整和甲烷三重整作為研究的體系。實驗中使用統(tǒng)一的Ni/MgAl2O4催化劑,甲烷重整工藝的模擬通過FSM-3060催化劑評價裝置和氣相色譜SP-6890聯(lián)用的方式實現(xiàn),在此裝置中完成反應(yīng)溫度、原料氣配比、空速對甲烷重整體系反應(yīng)性能的影響的考察,根據(jù)轉(zhuǎn)化率和選擇性結(jié)果,總結(jié)實驗規(guī)律并分析原因,并將各甲烷重整體系的實驗結(jié)果作進一步的對比分析,從中找出甲烷重整的有利條件和不利因素。主要結(jié)論如下： (1)通過對甲烷二氧化碳重整工藝條件的研究發(fā)現(xiàn)：甲烷和二氧化碳轉(zhuǎn)化率隨著反應(yīng)溫度的升高而升高,一氧化碳與氫氣選擇性則降低。隨著催化劑使用時間的延長,溫度越高各性能指標(biāo)下降速率越快,說明高溫不利于甲烷二氧化碳重整反應(yīng)； 隨著CH4/CO2配比的提高,甲烷轉(zhuǎn)化率和一氧化碳選擇性降低,二氧化碳轉(zhuǎn)化率和氫氣選擇性升高；隨著空速的提高,甲烷、二氧化碳轉(zhuǎn)化率和氫氣、一氧化碳選擇性下降,說明空速對屬于慢反應(yīng)的甲烷二氧化碳重整反應(yīng)影響較為明顯。甲烷二氧化碳重整所制備的合成氣中H2/CO體積比基本小于1,只有當(dāng)CH4/CO2配比較高時,H2/CO體積比才出現(xiàn)大于1的情況。 (2)通過對甲烷二氧化碳臨氧重整工藝條件的研究發(fā)現(xiàn)：甲烷、二氧化碳轉(zhuǎn)化率隨著反應(yīng)溫度的增加逐漸增加,尤其是低溫條件下反應(yīng)物轉(zhuǎn)化率相比甲烷二氧化碳重整有明顯的改善,說明氧氣的加入有利于反應(yīng)物轉(zhuǎn)化率的提升。但高溫條件下,反應(yīng)物轉(zhuǎn)化率和一氧化碳選擇性隨反應(yīng)的進行依然下降較快,體系的穩(wěn)定性依然較差。 隨著C02/02配比的提高,甲烷轉(zhuǎn)化率和H2/CO體積比逐漸下降,二氧化碳轉(zhuǎn)化率則逐漸提高,氫氣和一氧化碳選擇性出現(xiàn)增長；隨著空速的增加,甲烷和二氧化碳轉(zhuǎn)化率快速下降,產(chǎn)物選擇性則出現(xiàn)增長。 (3)通過對甲烷三重整工藝條件的研究發(fā)現(xiàn)：隨著反應(yīng)溫度的提高,反應(yīng)物轉(zhuǎn)化率相應(yīng)增加,一氧化碳選擇性和H2/CO體積比則降低。當(dāng)溫度為1073K,催化劑使用12h后,反應(yīng)物轉(zhuǎn)化率依然下降,但下降的幅度明顯弱于其他兩種體系,當(dāng)溫度較低時,體系穩(wěn)定性和高效性也要優(yōu)于另外兩種體系,說明水蒸氣形成消碳作用在一定程度上緩解了催化劑積炭效應(yīng),同時保留了反應(yīng)物高轉(zhuǎn)化率的特性。 甲烷和二氧化碳轉(zhuǎn)化率以及H2/CO體積比都隨著O2/H2O配比的增加而增加,一氧化碳選擇性則降低�？账俚奶岣呓档土朔磻�(yīng)物轉(zhuǎn)化率,但是提高了產(chǎn)物選擇性。
[Abstract]:In view of the outstanding environmental problems in China , the use of coal and petroleum as the source of energy is not in accord with the development of the national conditions . Therefore , the clean methane energy source is concerned , especially the methane - carbon dioxide reforming shows good environmental benefits and economic benefits in the preparation of synthesis gas , but the problem of catalyst carbon deposition makes the technology impossible to realize large - scale industrialization , and a large number of scientific research workers are starting from the research direction of the anti - carbon performance of the promotion catalyst , but are still in the experimental research stage .

In this experiment , the advantages of methane partial oxidation reforming and methane steam reforming are considered to improve the performance of methane carbon dioxide reforming reaction .

( 1 ) The conversion rate of methane and carbon dioxide is increased with the increase of the reaction temperature , and the selectivity of carbon monoxide and hydrogen is decreased .


With the increase of CH4 / CO2 ratio , methane conversion rate and carbon monoxide selectivity decrease , carbon dioxide conversion rate and hydrogen selectivity increase ;
With the increase of space velocity , the conversion of methane , carbon dioxide and hydrogen and carbon monoxide selectivity decrease , it is indicated that the effect of airspeed on methane carbon dioxide reforming reaction with slow reaction is more obvious . The H2 / CO volume ratio in the synthesis gas produced by methane carbon dioxide reforming is less than 1 , and only when CH4 / CO2 ratio is high , the H2 / CO volume ratio appears more than 1 .

( 2 ) The conversion of methane and carbon dioxide is increased with the increase of the reaction temperature , especially at low temperature . The conversion rate of the reactants and the selectivity of carbon monoxide are still decreased with the reaction , and the stability of the system is still poor .

With the increase of the ratio of CO2 / 02 , the conversion of methane and the ratio of H2 / CO volume gradually decreased , the conversion rate of carbon dioxide increased gradually , and the selectivity of hydrogen and carbon monoxide increased ;
With the increase of space velocity , the conversion rate of methane and carbon dioxide decreased rapidly , and the selectivity of products increased .

( 3 ) With the increase of reaction temperature , the conversion rate of the reactants increased correspondingly , the selectivity of carbon monoxide and the ratio of H2 / CO volume decreased . When the temperature was 1073K , the conversion rate of the reactants decreased , but the decrease was obviously weaker than that of the other two systems . When the temperature was lower , the stability and the efficiency of the system were better than that of the other two systems .

the conversion rate of methane and carbon dioxide and the H2 / CO volume ratio increase with the increase of the ratio of O2 / H2O , the selectivity of carbon monoxide is reduced , and the conversion rate of the reactants is reduced , but the selectivity of the product is improved .

【學(xué)位授予單位】：安徽理工大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：TE665.3

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