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氮化物在加氫催化劑表面的吸附_本科畢業(yè)設計論文-資料下載頁

2024-08-28 10:28本頁面

【導讀】形式存在,主要有兩種結構類型,非堿性吡咯類型和堿性吡啶類型。這一前沿領域的研究還可以優(yōu)化油氣開發(fā)方案,為提高油氣的最終采。收率帶來顯著的經濟效益。所以本課題對比較典型的含氮雜環(huán)化合物一吡??┑奈叫袨榧拔綑C理的研究具有一定的意義??┰贛oS2上吸附的3D圖,觀察其吸附位置,從而得到吸附機理。型,垂直吸附是吸附在N原子上,平行吸附是吸附在C=C上。附比垂直吸附更穩(wěn)定。

  

【正文】 J]. Analytical. Chemistry., 1934,510:4262. [12] Ball J S. Nitrogen pounds in petroleum[J]. Acs , 1962,42:2730. [13] Snyder L. Petroleum nitrogen pounds and oxygen pounds[J]. Acct. Che. Res., 1970,3:290299. [14] Bakel A J, Philp R P. The distribution and quantitation ofanitrogen pounds in crude oils and rock pyrolysates[J]. Organic Geochemistry,1990,16:233367. [15] Later D W, Lee M L,Bartle K D,et al. Chemical class separation and characterization of anic pounds in synthetic fuels[J]. Analytical. Chemistry,1981,53:16121620. [16] Richter F P, Caesar P D, Meisel S L,et al. Distribution ofnitrogen in petroleum according to basicity[J]. Industrial andEngineering Chemistry, 1952,44:26012605. [17] Ball J S, Whisman M L, Wenger W J. Nitrogen content ofpetroleums[J]. Industrial and Engineering Chemistry, 1951,4:25572581. 山東科技大學本科畢業(yè)設計(論文) 36 [18] Larter S R B F J, Bowler M, Li M. Chen,et al. Molecularindicators of secondary oil migration distances[J]. GeologicalSurvey of Canada, Calgary. Canada Nature, 1996,383:593597. [19] Charlesworth J M. Interaction of clay minerals with aniitrogen pounds released by kerogen pyrolsis[J]. Geochemistry et Cosmochimica Acta, 1986, 50:14311435. [20] Snyder L R. Principles of Adsorption Chromatography[M].London: Edward Arnold (publishers), Ld., 1968. [21] Frolov Y B, Smirnov M B, Vanyukova N A,et al. Carbazoles of crude oil[J]. Petroleum Chemistry USSR, 1989, 29:87102. [22] Van Duin A CT,larter S R. Aplication of molecular dynamicsin the prediction of dynamical molecular properties[J]. Organic Geochemistry :10431050. [23] 徐永昌 ,劉文匯 ,沈平 ,等 .天然氣地球化學的重要分支 —— 稀有氣體氣體地球化學 [J].天然氣地球科學 ,2020,14(3):157166. [24] 吡咯 .中國化工制造網 [引用日期 20200128]. [25] 金國干 .加氫催化劑生產線工藝流程草圖 [G].1997. [26] 徐龍伢 .催化劑制備方法 ,課件 [G].2020. [27] 朱洪法 ,劉麗芝 .催化劑載體制備及應用技術 [M].北京 :中國石化出版社 ,2020. [28] 李岳君 ,余立輝 .煉油催化劑生產技術 [M].北京 :中國 石化出版社, 2020. [29] 方向晨 .加氫精制 [M].北京 :中國石化出版社 ,2020. 山東科技大學本科畢業(yè)設計(論文) 37 [30] Solmm . [J],1991,302(1):31~46 [31] Quan Liyan(全麗艷 ),Lv Gongxuan(呂功煊 ). Catal(分子催化 ) [J],2020,19(5):376~381 [32] ,.,66,c23 (1974). [33] 吳茜薇 1裂解氣相色譜和聯(lián)用技術在高 分子材料研究中的應用 [J]1材料工程 , 1996, (8)1 山東科技大學本科畢業(yè)設計(論文) 38 致謝 非常 感謝 韓姝娜老師 ,本課題的研究工作是在 韓老 師的悉心指導下完成的。在整個課題的選題、探究實驗方案、數(shù)據分析和論文撰寫過程中,都是在韓 老師的精心指導和幫助 下完成 。 幾個月來 , 韓 老師淵博的學識、嚴謹?shù)闹螌W態(tài)度、活躍的學術思想、敏銳的洞察力以及認真負責的工作作風,讓我我獲益匪淺。在此論文即將完成之際,向 韓 老師致以最崇高的敬意和最衷心的感謝 ! 另外還要感謝與我同組同學的幫助,在與他們的探討中和他們的幫助下,學到了很多專業(yè)知 識和小常識,特別是在 Material Studio 軟件模擬方面,得到他們很大的幫助。 山東科技大學本科畢業(yè)設計(論文) 39 英文文獻 First principles study of heavy oil anonitrogen adsorption on NiMoS hydrotreating catalysts Abstract The adsorption of quinoline, acridine, indole, and carbazole on the welldefined NiMoS hydrotreating catalyst edge surface has been studied by means of densityfunctional theory (DFT) using a periodic supercell model. Quinoline and acridine, the basic nitrogencontaining molecules present in heavy oils, are preferably adsorbed on the Niedge surface through the lone pair electrons of the nitrogen atom, which produces relatively high adsorption energies (△Ea= 16–26 kcal mol1 ). Indole and carbazole, the nonbasic nitrogencontaining molecules, primarily interact with the NiMoS catalyst edge surface through the πelectrons of the carbon atoms. While indole preferentially adsorbs on the NiMoS surface through the βcarbon of the pyrrolic ring (△Ea= 19 kcal mol1 ), carbazole primarily interacts with the NiMoS surface through the phenyl rings (△Ea = 13 kcal mol1). The relative adsorptivities and energetically preferred adsorption modes of the nitrogencontaining molecules in heavy oils can 山東科技大學本科畢業(yè)設計(論文) 40 provide insights into experimental observations about hydrodenitrogenation (HDN) kiics and reaction pathways. Keywords: Adsorption。 NiMoS。 Hydrodenitrogenation。 Quinoline。 Indole。 Acridine carbazole。 Heavy oil。 Densityfunctional theory 1. Introduction The increasing demand for processing heavy oils and vacuum residue, which contain significantly more nitrogen pounds than conventional light crude oils, requires the development of hydrotreating catalysts with higher hydrodenitrogenation (HDN) activity. In order to develop new hydrotreating catalysts with high activity to remove refractory nitrogen pounds present in heavy oils, a detailed understanding of HDN catalysis, including the structure of the catalysts, the electronic configurations of the nitrogen pounds, and the adsorption and reaction mechanisms of basic and nonbasic nitrogen pounds on catalyst surfaces, is required. Molybdenumbased sulfides are widely used in the oil refining industry as hydrotreating catalysts to remove sulfur and nitrogen from heavy oils. The active phase on these hydrotreating catalysts has a MoS2like structure, and active sites are located at edge surfaces of the MoS2[1,2]. Due to extensive experimental and theoretical research, a good understanding of the structure of the active phase at the atomic level and the location of promoters (nickel and cobalt) in the active phase has been achieved. For unpromoted MoS2, the( ?010) Sedge and( 10 ?0) Moedge are normally covered by bridge sulfur 山東科技大學本科畢業(yè)設計(論文) 41 atoms and have very few sulfur vacancies at reaction conditions[3–5]. In the promoted catalysts, cobalt prefers to incorporate into the Sedge and nickel to the Moedge of MoS2 , and the promoted edge surfaces have more vacant sites under typical hydrotreating reaction conditions[6–8]. Most nitrogen present in heavy crude oils is in the form of heterocyclic anonitrogen pounds containing basic (pyridinic) or nonbasic (pyrrolic) ring structures[9]. Non basic nitrogen pounds are a significant fraction of the total nitrogen content in heavy oils[10,11]. These nonbas
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