以芳烃萘作为参照物，研究了超大比表面积活性炭 MSC-30对喹啉、吲哚和咔唑的吸附选择性。进一步采用3种不同的氧化改性方法对 MSC-30活性炭进行了氧化改性，考察氧化改性对活性炭吸附脱氮选择性的影响。结果表明，该活性炭及氧化改性样品选择性吸附脱氮。氧化改性后，活性炭对氮化物的选择性进一步提高，并且对氮化物的吸附量增加。通过量子化学密度泛函理论(DFT)对目标吸附质的前线轨道能量分布进行计算，结果证明，活性炭对于氮化物的吸附选择性高于对芳烃萘的选择性，这和吸附质的反应活泼顺序一致。氧化改性的活性炭，由于表面含氧基团增加，不利于吸附稳定的萘，而有利于吸附较活泼的吲哚和喹啉，尤其倾向于吸附碱性氮化物喹啉。在强氧化的活性炭样品 MSC-N 和 MSC-NS 上，喹啉的吸附量分别高达1.05和1.06mmol/g。
This work examines the adsorptive selectivity of activated carbon (AC)MSC-30 for the nitrogen com-pounds,quinoline,indole and carbazole,based on aromatic naphthalene as reference compound.Furthermore, the effects of three different oxidation modification methods on the adsorptive selectivity of AC were investiga-ted.It was found that both of original and modified ACs selectively adsorbed nitrogen compounds.Oxidation modification of AC further improved the selectivity for nitrogen compounds as well as the adsorption capacity of nitrogen compounds.The frontier orbital distribution of target adsorbates was calculated through the density functional theory (DFT)method.The results demonstrated that the higher selectivity for nitrogen compounds than that for aromatic naphthalene was consistent with the order of adsorbates'reaction activities.Moreover, due to the increased surface oxygen-containing groups on oxidized activated carbon,they weren’t beneficial to adsorb stable naphthalene,but favored adsorbing indoles and quinoline,especially tended to adsorb basic quino-line.The adsorptive capacity for quinoline on severely oxidized samples MSC-N and MSC-NS could reach 1.05 and 1.06mmol/g,respectively.
参考文献
| [1] | Edward F;Franklin M .Hydrodenitrogenation of petrole-um[J].Catalysis Reviews:Science and Engineering,2005,47(03):297-489. |
| [2] | Song Chunshan .An overview of new approaches to deep desulfurization for ultra-clean gasoline,diesel fuel and j et fuel[J].Catalysis Today,2003,86(01):211-263. |
| [3] | Xiaoling Ma;Lu Sun .A new approach to deep desulfurization of gasoline, diesel fuel and jet fuel by selective adsorption for ultra-clean fuels and for fuel cell applications[J].Catalysis Today,2002(1/2):107-116. |
| [4] | Yang Hong;Chen Jinwen;Yevgenia B et al.Effect of nitrogen removal from light cycle oil on the hydrodesul-phurization of dibenzothiophene,4-methyldibenzothio-phene and 4,6-dimethyldibenzothiophene[J].Catalysis Today,2005,109(01):16-23. |
| [5] | Georgina L;Antonio D L R;Luis C et al.Inhibition effects of nitrogen compounds on the hydrodesulfurization of dibenzothiophene[J].Applied Catalysis A:General,2001,207(01):103-112. |
| [6] | Michael G;Bruce G .Reactivities,reaction networks,and kinetics in high-pressure catalytic hydroprocessing[J].In-dustrial and Engineering Chemistry Research,1991,30(09):2021-2058. |
| [7] | Sonja E;De Beer V H J;Prins R .Hydrodenitrogenation of quinoline over carbon-supported transition-metal sul-fides[J].Journal of Catalysis,1991,127(02):619-630. |
| [8] | Liao, P.;Yuan, S.;Xie, W.;Zhang, W.;Tong, M.;Wang, K..Adsorption of nitrogen-heterocyclic compounds on bamboo charcoal: Kinetics, thermodynamics, and microwave regeneration[J].Journal of Colloid and Interface Science,2013:189-195. |
| [9] | Imteaz Ahmed;Zubair Hasan;Nazmul Abedin Khan.Adsorptive denitrogenation of model fuels with porous metal-organic frameworks (MOFs): Effect of acidity and basicity of MOFs[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2013:123-129. |
| [10] | Georgina C. Laredo;Pedro M. Vega-Merino;Fernando Trejo-Zarraga.Denitrogenation of middle distillates using adsorbent materials towards ULSD production: A review[J].Fuel Processing Technology,2013:21-32. |
| [11] | Jae Hyung Kim;Xiaoliang Ma;Anning Zhou;Chunshan Song .Ultra-deep desulfurization and denitrogenation of diesel fuel by selective adsorption over three different adsorbents:A study on adsorptive selectivity and mechanism[J].Catalysis Today,2006(1/2):74-83. |
| [12] | Masoud Almarri;Xiaoliang Ma;Chunshan Song .Selective Adsorption for Removal of Nitrogen Compounds from Liquid Hydrocarbon Streams over Carbon- and Alumina-Based Adsorbents[J].Industrial & Engineering Chemistry Research,2009(2):951-960. |
| [13] | 夏启斌,余谟鑫,姬乔娜,方媛,李忠.超大比表面积活性炭对柴油中噻吩类硫化物的吸附性能[J].功能材料,2009(10):1730-1733. |
| [14] | 余谟鑫,李忠,奚红霞,夏启斌,王书文.椰壳类活性炭孔隙结构对苯并噻吩脱附活化能的影响[J].功能材料,2007(10):1664-1668. |
| [15] | 文婕,孙文晶,杨文,王宁,储伟.氧化活性炭在模型油中吸附脱氮性能研究[J].功能材料,2012(13):1770-1773,1777. |
| [16] | Zielke U.;Hoffman WP.;Huttinger KJ. .SURFACE-OXIDIZED CARBON FIBERS .1. SURFACE STRUCTURE AND CHEMISTRY[J].Carbon: An International Journal Sponsored by the American Carbon Society,1996(8):983-998. |
| [17] | Chang Yu;Jie Shan Qiu;Yu Feng Sun;Xian Hui Li;Gang Chen;Zong Bin Zhao .Adsorption removal of thiophene and dibenzothiophene from oils with activated carbon as adsorbent: effect of surface chemistry[J].Journal of porous materials,2008(2):151-157. |
| [18] | Morenocastilla C.;Mueden A.;Carrascomarin F. .THE CREATION OF ACID CARBON SURFACES BY TREATMENT WITH (NH4)(2)S2O8[J].Carbon: An International Journal Sponsored by the American Carbon Society,1997(10/11):1619-1626. |
| [19] | Anning Zhou;Xiaoliang Ma;Chunshan Song .Effects of oxidative modification of carbon surface on the adsorption of sulfur compounds in diesel fuel[J].Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications,2009(3/4):190-199. |
| [20] | Abraham M;Amatzya M;Mordecai R .Paratropicity and antiaromaticity:role of the homo-lumo energy gap[J].Tetrahedron,1985,41(04):785-791. |
| [21] | Strelko VV.;Thrower PA.;Kuts VS. .On the mechanism of possible influence of heteroatoms of nitrogen, boron and phosphorus in a carbon matrix on the catalytic activity of carbons in electron transfer reactions[J].Carbon: An International Journal Sponsored by the American Carbon Society,2000(10):1499-1503. |
| [22] | Zhang M.;Kan YH.;Zang OJ.;Su ZM.;Wang RS. .Why silicon nanotubes stably exist in armchair structure?[J].Chemical Physics Letters,2003(1/2):81-86. |
- 下载量()
- 访问量()
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%