介質(zhì)阻擋放電和火花放電轉(zhuǎn)化甲烷的研究
發(fā)布時(shí)間：2018-12-17 19:06
【摘要】：隨著石油資源的日益枯竭和環(huán)境問(wèn)題日益嚴(yán)重,以CH4為原料生產(chǎn)化學(xué)品的新途徑越來(lái)越受到國(guó)內(nèi)外學(xué)者的廣泛關(guān)注。本文主要進(jìn)行低溫等離子體甲烷轉(zhuǎn)化制高碳烴和甲烷重整制合成氣的研究,并重點(diǎn)對(duì)比了介質(zhì)阻擋放電和火花放電兩種放電形式對(duì)于甲烷轉(zhuǎn)化的差異。得到如下結(jié)果和結(jié)論：在甲烷轉(zhuǎn)化制高碳烴的研究中,介質(zhì)阻擋放電條件下產(chǎn)物分布范圍較廣,主要產(chǎn)物為C2H6、C3H8和C4H1o飽和烷烴,選擇性分別為46.9%、23.4%和14.2%,系統(tǒng)考察了進(jìn)料流量、放電功率、放電間距、填充介質(zhì)對(duì)甲烷轉(zhuǎn)化率和產(chǎn)物選擇性的影響,結(jié)果表明減小甲烷進(jìn)料流量、提高放電功率、減小放電間距、填充小顆粒介質(zhì)均能夠提高甲烷轉(zhuǎn)化率,并在一定程度上調(diào)節(jié)產(chǎn)物分布�；鸹ǚ烹娹D(zhuǎn)化甲烷所得的主要產(chǎn)物為C2H2,其選擇性超過(guò)95%,但是火花放電積碳快,放電穩(wěn)定性較差；通過(guò)添加H2、N2、Ar、He、02和NH3等添加氣得出：H2、He和NH3對(duì)C2烴的分布具有一定調(diào)節(jié)作用,02對(duì)CH4沒有氧化偶聯(lián)作用,但它可通過(guò)生成CO而顯著影響產(chǎn)物分布；Ar、He、H2會(huì)提高甲烷火花放電的轉(zhuǎn)化能量效率,02、N2和NH3會(huì)降低CH4火花放電的轉(zhuǎn)化能量效率；添加H2和02能夠延緩積碳速度,提高放電穩(wěn)定性,相比之下,02添加氣對(duì)改善放電穩(wěn)定性的效果最好。最后通過(guò)產(chǎn)物分析和發(fā)射光譜(OES)數(shù)據(jù),推斷出介質(zhì)阻擋放電和火花放電轉(zhuǎn)化甲烷可能的活化途徑。甲烷轉(zhuǎn)化制合成氣的研究中,在反應(yīng)物的轉(zhuǎn)化率和合成氣(CO+H2)產(chǎn)物選擇性方面,火花放電都要優(yōu)于介質(zhì)阻擋放電。CH4-CO2火花放電制合成氣時(shí)存在反應(yīng)器積碳問(wèn)題,反應(yīng)不能長(zhǎng)時(shí)間穩(wěn)定進(jìn)行,添加02能夠徹底擺脫CH4-CO2火花放電制合成氣時(shí)的反應(yīng)器結(jié)炭問(wèn)題,而且CH4-O2-CO2三組分氣體火花放電制合成氣方法能通過(guò)改變?nèi)N反應(yīng)氣體的進(jìn)料比例而靈活調(diào)節(jié)產(chǎn)物H2/CO比。在CH4流量20 mL/min、O2流量10mL/min、CO2流量12.38 mL/min、注入功率為28W的條件下進(jìn)行的CH4-O2-CO2火花放電連續(xù)運(yùn)轉(zhuǎn)實(shí)驗(yàn),在所考察的100 h內(nèi),CH4、CO2的轉(zhuǎn)化率穩(wěn)定,其平均值分別為61.73%和32.39%,產(chǎn)物中H2/CO的比例保持在1.0左右；在CH4流量20 mL/min、O2流量10mL/min、CO2流量0.77 mL/min、注入功率為28 W的條件下進(jìn)行的CH4-O2-CO2火花放電連續(xù)運(yùn)轉(zhuǎn)實(shí)驗(yàn),在所考察的100 h內(nèi),CH4、CO2的轉(zhuǎn)化率穩(wěn)定,其平均值分別為63.87%和37.50%,產(chǎn)物中H2/CO的比例保持在2.0左右。
[Abstract]:With the increasingly depletion of petroleum resources and the increasingly serious environmental problems, the new way to produce chemicals using CH4 as raw material has attracted more and more attention from domestic and foreign scholars. In this paper, the methane conversion from low temperature plasma to high carbon hydrocarbon and methane reforming to syngas are studied, and the differences between dielectric barrier discharge and spark discharge for methane conversion are compared. The results and conclusions are as follows: in the study of methane conversion to high carbon hydrocarbons, the distribution range of the products under dielectric barrier discharge is relatively wide. The main products are C _ 2H _ 6C _ 3H _ 8 and C4H1o saturated alkanes with selectivity of 46.9, respectively. The effects of feed flow rate, discharge power, discharge spacing and filling medium on methane conversion and product selectivity were investigated systematically. The results showed that the feed flow rate of methane was reduced, the discharge power was increased, and the discharge distance was reduced. Filling with small particle media can increase methane conversion and adjust the distribution of products to some extent. The main product of methane conversion from spark discharge is C _ 2H _ 2, its selectivity is more than 95%, but the spark discharge has fast carbon accumulation and poor discharge stability. By adding H _ 2H _ 2N _ 2N _ 2H _ 2H _ 2O _ 2 and NH3 gas, it was found that H _ 2H _ 2H _ 2 and NH3 could regulate the distribution of C _ 2 hydrocarbon to some extent, and that O _ 2 had no oxidative coupling effect on CH4, but it could significantly influence the distribution of products by forming CO. Ar,He,H2 can improve the conversion energy efficiency of methane spark discharge, while 02 N 2 and NH3 can decrease the conversion energy efficiency of CH4 spark discharge. The addition of H2 and 02 can delay the carbon deposition rate and improve the discharge stability. Finally, the possible activation pathways of methane conversion from dielectric barrier discharge and spark discharge were inferred by product analysis and emission spectrum (OES) data. In the research of methane conversion to syngas, the spark discharge is superior to dielectric barrier discharge in the conversion of reactants and the selectivity of CO H2 products. The reaction can not be carried out stably for a long time. Adding 02 can completely get rid of the problem of reactor coking when CH4-CO2 spark discharge is used to produce syngas. Moreover, the CH4-O2-CO2 three-component gas spark discharge method can flexibly adjust the H2/CO ratio by changing the feed ratio of the three reaction gases. The continuous operation experiment of CH4-O2-CO2 spark discharge was carried out under the condition of CH4 flow rate of 20 mL/min,O2, flow rate of 10 mL / min CO 2 flow rate of 12.38 mL/min, injection power of 28 W, and the conversion rate of CH4,CO2 was stable within 100 h. The average values were 61.73% and 32.39%, respectively, and the proportion of H2/CO in the product remained about 1.0. The continuous operation experiment of CH4-O2-CO2 spark discharge was carried out under the condition of CH4 flow rate of 20 mL/min,O2, flow rate of 10 mL / min CO 2 flow rate of 0.77 mL/min, injection power of 28 W, and the conversion rate of CH4,CO2 was stable within 100 h. The average values were 63.87% and 37.50%, respectively, and the proportion of H2/CO in the product remained about 2.0.
【學(xué)位授予單位】：大連理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TE665.3
本文編號(hào)：2384668
[Abstract]:With the increasingly depletion of petroleum resources and the increasingly serious environmental problems, the new way to produce chemicals using CH4 as raw material has attracted more and more attention from domestic and foreign scholars. In this paper, the methane conversion from low temperature plasma to high carbon hydrocarbon and methane reforming to syngas are studied, and the differences between dielectric barrier discharge and spark discharge for methane conversion are compared. The results and conclusions are as follows: in the study of methane conversion to high carbon hydrocarbons, the distribution range of the products under dielectric barrier discharge is relatively wide. The main products are C _ 2H _ 6C _ 3H _ 8 and C4H1o saturated alkanes with selectivity of 46.9, respectively. The effects of feed flow rate, discharge power, discharge spacing and filling medium on methane conversion and product selectivity were investigated systematically. The results showed that the feed flow rate of methane was reduced, the discharge power was increased, and the discharge distance was reduced. Filling with small particle media can increase methane conversion and adjust the distribution of products to some extent. The main product of methane conversion from spark discharge is C _ 2H _ 2, its selectivity is more than 95%, but the spark discharge has fast carbon accumulation and poor discharge stability. By adding H _ 2H _ 2N _ 2N _ 2H _ 2H _ 2O _ 2 and NH3 gas, it was found that H _ 2H _ 2H _ 2 and NH3 could regulate the distribution of C _ 2 hydrocarbon to some extent, and that O _ 2 had no oxidative coupling effect on CH4, but it could significantly influence the distribution of products by forming CO. Ar,He,H2 can improve the conversion energy efficiency of methane spark discharge, while 02 N 2 and NH3 can decrease the conversion energy efficiency of CH4 spark discharge. The addition of H2 and 02 can delay the carbon deposition rate and improve the discharge stability. Finally, the possible activation pathways of methane conversion from dielectric barrier discharge and spark discharge were inferred by product analysis and emission spectrum (OES) data. In the research of methane conversion to syngas, the spark discharge is superior to dielectric barrier discharge in the conversion of reactants and the selectivity of CO H2 products. The reaction can not be carried out stably for a long time. Adding 02 can completely get rid of the problem of reactor coking when CH4-CO2 spark discharge is used to produce syngas. Moreover, the CH4-O2-CO2 three-component gas spark discharge method can flexibly adjust the H2/CO ratio by changing the feed ratio of the three reaction gases. The continuous operation experiment of CH4-O2-CO2 spark discharge was carried out under the condition of CH4 flow rate of 20 mL/min,O2, flow rate of 10 mL / min CO 2 flow rate of 12.38 mL/min, injection power of 28 W, and the conversion rate of CH4,CO2 was stable within 100 h. The average values were 61.73% and 32.39%, respectively, and the proportion of H2/CO in the product remained about 1.0. The continuous operation experiment of CH4-O2-CO2 spark discharge was carried out under the condition of CH4 flow rate of 20 mL/min,O2, flow rate of 10 mL / min CO 2 flow rate of 0.77 mL/min, injection power of 28 W, and the conversion rate of CH4,CO2 was stable within 100 h. The average values were 63.87% and 37.50%, respectively, and the proportion of H2/CO in the product remained about 2.0.
【學(xué)位授予單位】：大連理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2015
【分類號(hào)】：TE665.3
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