过渡金属离子改性Na-13X分子筛对噻吩类硫化物的吸附性能与机理Adsorption of Thiophenic Sulfur in Transition Metal Ion Modified Na-13X Zeolites
周林,彭安忠,居沈贵
摘要(Abstract):
采用液相离子交换法制备Cu+-13X、Ni2+-13X和Co2+-13X吸附剂,利用XRD、FT-IR和Laser-raman等对其进行表征。在常温常压条件下,以含有噻吩、2-乙基噻吩和苯并噻吩的正己烷溶液为模拟汽油,通过静态吸附实验与动力学吸附实验研究了3种吸附剂对噻吩、2-乙基噻吩和苯并噻吩的吸附性能与机理,并采用Langmuir模型对静态吸附平衡数据进行拟合和Crank单孔扩散模型对动力学吸附数据进行拟合。实验结果表明过渡金属离子改性的分子筛对噻吩类硫化物有较高的吸附含量;改性后分子筛的选择吸附性能取决于吸附质与吸附剂之间的π络合作用和吸附剂的表面酸性,而受硫化物的空间位阻影响作用很小。
关键词(KeyWords): 过渡金属离子;脱硫;π络合;噻吩类硫化物
基金项目(Foundation): 国家自然科学基金(21176118)
作者(Author): 周林,彭安忠,居沈贵
参考文献(References):
- [1]KE Ming(柯明),ZHOU Ai-guo(周爱国),ZHAO Zhen-sheng(赵振盛),et al.Alkylation of thiophenic sulfur technology in the production of clean fuel(FCC汽油烷基化脱硫技术进展)[J].Chemical Industry and Engineering Progress(化工进展),2006,25(4):357-361.
- [2]JU Shen-gui(居沈贵),ZENG Yong-ping(曾勇平),YAO Hu-qing(姚虎卿).Unconventional desulfurization technology(非常规汽油脱硫技术)[J].Modern Chemical Industry(现代化工),2004,24(1):56-59.
- [3]Liu B J,Zhu Y B,Liu S W,et al.Adsorption equilibrium of thiophenic sulfur compounds on the Cu-BTC metal-organic framework[J].J Chem Eng Data,2012,57(4):1326-1330.
- [4]SONG Li-juan(宋丽娟),PAN Ming-xue(潘明雪),QIN Yu-cai(秦玉才),et al.The adsorptive properties and mechanism of Na Y zeolites(Ni Y分子筛选择性吸附脱硫性能及作用机理)[J].Chem J Chinese Universities(高等学校化学学报),2011,3(32):787-792.
- [5]DAI Su-juan(代素绢),CHEN Hui-juan(陈慧娟),HAN Xue-lian(韩雪莲).The influence of different adsorbents on the deep desulfurization(不同吸附剂对FCC汽油深度脱硫的影响)[J].J Northeast Petroleum University(东北石油大学学报),2005,29(4):55-58.
- [6]Yang R T,Hernánadez-Maldonado A J,Yang F H.Desulfurization of transportation fuels with zeolites under ambient conditions[J],Science,2003,301(5629):79-81.
- [7]Velu S,Ma X L,Song C S.Selective adsorption for removing sulfur from jet fuel over zeolite-based adsorbents[J].Industrial&Engineering Chemistry Research,2003,42(21):5293-5304.
- [8]DUAN Lin-hai(段林海),MENG Xiu-hong(孟秀红),SHI Yan(施岩),et al.Selective adsorption desulfurization performance and mechanism of sulfur compounds over modified Y zeolite(不同硫化物在改性Y分子筛上的选择性吸附脱硫性能及机理)[J].Acta Petrolei Sinica(Petroleum Processing Section)(石油学报(石油化工)),2009(S):74-80.
- [9]Dastanian M,Seyedeyn-Azad F.Desulfurization of gasoline over nanoporous nickel-loaded Y-type zeolite at ambient conditions[J].Ind Eng Chem Res,2010,49(22):11254-11259.
- [10]Hiroshi Kitagawa(北川浩),Suzuki Ichiro(铃木谦一郎),LU Zheng-li(鹿政理)译.Adsorption basis and design(吸附的基础与设计)[M].Beijing(北京):Chemical Industry Press(化学工业出版社),1983.
- [11]TIAN Fu-ping(田福平),WU Wei-cheng(吴维成),JIANG Zong-xuan(蒋宗轩),et al.Cu Na Y zeolite on the selective absorption of sulfur components in gasoline and its IR spectroscopy(Cu Na Y分子筛上汽油馏分中含硫组分的选择吸附及其红外光谱研究)[J].Chem J Chinese Universities(高等学校化学学报),2005,26(12):2351-2353.
- [12]Garcia L,Lercher J A.Adsorption and surface reactions of thiophene on ZSM-5 zeolites[J].J Physical Chemistry,1992,96(6):2669-2675.
- [13]WU Ya-juan(吴亚娟).The effect of alkyl electronic(烷基的电子效应)[J].Textile Basic Science Journal(纺织基础科学学报),1994,7(3):257-261.
- [14]YANG Xian-chun(杨先春),LU Wan-zhen(陆婉珍),ZHAO Bi-Ying(赵壁英),et al.Measurement of surface L acid and B acid by laser raman sperctroscopic(用激光喇曼光谱法定最测定表面L酸和B酸量)[J].Petrochemical Technology(石油化工),1991,30(5):340-344.
- [15]YANG Xian-chun(杨先春),CHEN Qing-feng(陈青峰),ZHAO Bi-ying(赵壁英).Laser raman sperctroscopic investigation surface sites of acidic type on solid catalysts by adsorbed pyridine(固体催化剂表面酸类型的激光喇曼光谱特性研究)[J].J of Light Scatting(光散射学报),1991,3(12):32-40.
- [16]Shi Y C,Yang X J,Tian F P.Effects of toluene on thiophene adsorption over Na Y and Ce(IV)Y zeolites[J].J Natural Gas Chemistry,2012,21(4):421-425.
- [17]YE Zheng-hua(叶振华).Chemical adsorption separation process(化工吸附分离过程)[M].Beijing(北京):China Petrochemical Press(中国石化出版社),1992.
- [18]Ruthven D M.Principles of adsorption and adsorption processes[M].New York:John Wiley and Sons Inc,1984:149-161.