本文選題：甲烷重整 + 工藝條件　； 參考：《安徽理工大學》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注,尤其甲烷二氧化碳重整在制備合成氣方面表現出良好的環(huán)境效益和經濟效益,但催化劑積炭問題使得此技術無法實現大規(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聯用的方式實現,在此裝置中完成反應溫度、原料氣配比、空速對甲烷重整體系反應性能的影響的考察,根據轉化率和選擇性結果,總結實驗規(guī)律并分析原因,并將各甲烷重整體系的實驗結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：甲烷和二氧化碳轉化率隨著反應溫度的升高而升高,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下降速率越快,說明高溫不利于甲烷二氧化碳重整反應； 隨著CH4/CO2配比的提高,甲烷轉化率和一氧化碳選擇性降低,二氧化碳轉化率和氫氣選擇性升高；隨著空速的提高,甲烷、二氧化碳轉化率和氫氣、一氧化碳選擇性下降,說明空速對屬于慢反應的甲烷二氧化碳重整反應影響較為明顯。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CH4/CO2配比較高時,H2/CO體積比才出現大于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：甲烷、二氧化碳轉化率隨著反應溫度的增加逐漸增加,尤其是低溫條件下反應物轉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物轉化率的提升。但高溫條件下,反應物轉化率和一氧化碳選擇性隨反應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,甲烷轉化率和H2/CO體積比逐漸下降,二氧化碳轉化率則逐漸提高,氫氣和一氧化碳選擇性出現增長；隨著空速的增加,甲烷和二氧化碳轉化率快速下降,產物選擇性則出現增長。 (3)通過對甲烷三重整工藝條件的研究發(fā)現：隨著反應溫度的提高,反應物轉化率相應增加,一氧化碳選擇性和H2/CO體積比則降低。當溫度為1073K,催化劑使用12h后,反應物轉化率依然下降,但下降的幅度明顯弱于其他兩種體系,當溫度較低時,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,同時保留了反應物高轉化率的特性。 甲烷和二氧化碳轉化率以及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镛D化率,但是提高了產物選擇性。
[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 .

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

【參考文獻】

相關期刊論文 前10條

1 王銳;劉雪斌;陳燕馨;李文釗;徐恒泳;;金屬-載體相互作用對CH_4/CO_2重整反應中Rh基催化劑抗積炭性能的影響[J];催化學報;2007年10期

2 Ahmed S.A.AL-FATESH;Anis H.FAKEEHA;Ahmed E.ABASAEED;;助劑對甲烷干重整 Ni/γ-Al_2O_3催化劑性能的影響(英文)[J];催化學報;2011年10期

3 李洪強;洪慧;金紅光;蔡睿賢;;天然氣水蒸氣重整甲醇動力串聯型多聯產系統(tǒng)性能分析與優(yōu)化[J];工程熱物理學報;2011年02期

4 孫杰;孫春文;李吉剛;周添;董中朝;陳立泉;;甲烷水蒸氣重整反應研究進展[J];中國工程科學;2013年02期

5 井強山;方林霞;樓輝;鄭小明;;甲烷臨氧催化轉化制合成氣研究進展[J];化工進展;2008年04期

6 孫道安;李春迎;張偉;呂劍;;典型碳氫化合物水蒸氣重整制氫研究進展[J];化工進展;2012年04期

7 姜洪濤;李會泉;張懿;;甲烷三重整制合成氣[J];化學進展;2006年10期

8 翁維正,羅春容,李建梅,劉穎,林海強,黃傳敬,萬惠霖;Ir/SiO_2上甲烷部分氧化制合成氣反應的原位時間分辨紅外和原位Raman光譜表征[J];化學學報;2004年18期

9 胡久彪;余長林;周曉春;;甲烷部分氧化催化劑上的積碳研究進展[J];有色金屬科學與工程;2012年02期

10 王莉;敖先權;王詩瀚;;甲烷與二氧化碳催化重整制取合成氣催化劑[J];化學進展;2012年09期

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