【摘要】：瀝青質(zhì)的吸附和沉積是造成加氫催化劑結(jié)焦最主要的原因,故其在催化劑中擴散方面的研究日益受到重視。本文以塔河常壓渣油的瀝青質(zhì)為原料,甲苯為溶劑進行了擴散實驗。擴散實驗在不同實驗條件下進行,并使用MATLAB軟件編寫程序,將實驗數(shù)據(jù)和擴散模型擬合得到各個參數(shù)值,考察不同反應條件對瀝青質(zhì)聚集體在加氫催化劑中有效擴散系數(shù)的影響。將實驗數(shù)據(jù)和已知參數(shù)結(jié)合擴散受阻有關方程計算擴散受阻因子,以考察不同實驗條件下的擴散受阻因子和瀝青質(zhì)在不同催化劑中的擴散受阻程度。不同實驗條件下,瀝青質(zhì)在加氫催化劑中的有效擴散系數(shù)受到不同程度的影響。有效擴散系數(shù)隨溶液初始濃度的增加而減小,而且減小的幅度明顯降低;延長操作時間,有效擴散系數(shù)逐漸減小,并且減小的速度越來越快;當催化劑孔徑減小時,有效擴散系數(shù)減小,而且,由于瀝青質(zhì)聚集體在催化劑中的擴散受催化劑孔徑的影響較大,使得有效擴散系數(shù)隨孔徑變化的幅度較大。隨著操作時間的增加,催化劑孔道堵塞越來越嚴重,阻礙了瀝青質(zhì)聚集體的進一步擴散,使有效擴散系數(shù)逐漸減小,在相同擴散時間內(nèi),瀝青質(zhì)滲透深度增加的速度逐漸減小。瀝青質(zhì)在加氫催化劑中的擴散受阻因子受到不同實驗條件的影響。隨著溶液初始濃度的增加,瀝青質(zhì)在加氫催化劑孔道中擴散時的受阻程度增加,結(jié)合擴散實驗數(shù)據(jù)和相應數(shù)學模型計算出的擴散受阻因子減小。延長擴散時間,瀝青質(zhì)聚集體在催化劑表面和孔道中的吸附和沉積越來越嚴重,則催化劑孔徑和孔隙率減小,導致瀝青質(zhì)聚集體在催化劑中的擴散受阻因子減小。催化劑孔徑越小,瀝青質(zhì)聚集體在催化劑中的擴散受阻程度越大,則擴散受阻因子越小。瀝青質(zhì)聚集體在平均孔半徑為4.7nm的催化劑中的擴散受到嚴重阻礙,其擴散受阻因子F(λ)值非常小。
文內(nèi)圖片：
圖片說明：瀝青質(zhì)單元結(jié)構(gòu)
[Abstract]:The adsorption and deposition of asphaltene are the most important reasons for coking of hydrogenation catalysts, so more and more attention has been paid to the diffusion of asphaltenes in catalysts. In this paper, the asphaltene of Tahe atmospheric residue was used as raw material and toluene as solvent. The diffusion experiment was carried out under different experimental conditions, and the experimental data and diffusion model were fitted with MATLAB software to obtain each parameter value, and the effect of different reaction conditions on the effective diffusion coefficient of asphalt aggregates in hydrogenation catalyst was investigated. The diffusion blocking factor was calculated by combining the experimental data with known parameters with the equation of diffusion hindrance in order to investigate the diffusion blocking factor and asphaltene diffusion blocking degree in different catalysts under different experimental conditions. Under different experimental conditions, the effective diffusion coefficient of asphaltene in hydrogenation catalyst is affected to varying degrees. The effective diffusion coefficient decreases with the increase of the initial concentration of the solution, and the effective diffusion coefficient decreases with the increase of the initial concentration of the solution. When the pore size of the catalyst decreases, the effective diffusion coefficient decreases. Moreover, the effective diffusion coefficient varies greatly with the pore size of the catalyst because the diffusion of asphalt aggregates in the catalyst is greatly affected by the pore size of the catalyst. With the increase of operation time, the pore blockage of catalyst becomes more and more serious, which hinders the further diffusion of asphaltene aggregates, and the effective diffusion coefficient decreases gradually, and the rate of increase of asphaltene penetration depth decreases gradually in the same diffusion time. The diffusion blocking factor of asphaltene in hydrogenation catalyst is affected by different experimental conditions. With the increase of the initial concentration of the solution, the degree of hindrance of asphaltene diffusion in the pore of hydrogenation catalyst increases, and the diffusion hindrance factor calculated by combining the diffusion experimental data and the corresponding mathematical model decreases. When the diffusion time is prolonged, the adsorption and deposition of asphaltene aggregates on the surface and pores of the catalyst become more and more serious, and the pore size and porosity of the catalyst decrease, which leads to the decrease of the diffusion hindrance factor of the asphaltene aggregates in the catalyst. The smaller the pore size of the catalyst is, the greater the degree of diffusion hindrance of asphaltene aggregates in the catalyst is, the smaller the diffusion blocking factor is. The diffusion of asphalt aggregates in catalysts with average pore radius of 4.7nm is seriously hindered, and the diffusion blocking factor F (位) is very small.
【學位授予單位】：中國石油大學(華東)
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：TE624.9

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