四丙基氢氧化铵改性TS-1催化氧化脱除2-甲基噻吩  

CATALYTIC OXIDATIVE REMOVAL OF 2-METHYLTHIOPHENE OVER TS-1 MODIFIED BY TPAOH

作　　者：赵丽霞[1] 李钢[1] 金长子[1] 王云[1] 王祥生[1] 

机构地区：[1]大连理工大学精细化工国家重点实验室,辽宁大连116012

出　　处：《石油学报（石油加工）》2007年第4期95-99,共5页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家自然科学基金(20406005);高等学校全国优秀博士学位论文作者专项资金(200346);新世纪优秀人才支持计划(NCET-04-0270);中国石油天然气集团公司石油科技中青年创新基金(04E709)项目资助

摘　　要：采用有机碱四丙基氢氧化铵(TPAOH)对微米TS-1进行碱改性。以改性后的TS-1为催化剂,H2O2为氧化剂,对含有2-甲基噻吩的正辛烷模拟燃料进行氧化脱硫研究。采用XRD、UV-vis、TEM、N2物理吸附等手段对改性前后的样品进行表征。考察了TPAOH浓度、改性温度以及改性时间对微米TS-1氧化脱除2-甲基噻吩性能的影响。结果表明,与未改性的样品相比,改性后的TS-1骨架结构未发生明显变化,骨架钛和非骨架钛含量均有所降低,并且生成一些大小约为1.4nm和40～60nm的孔,比表面积和孔容增加。TPAOH改性TS-1对2-甲基噻吩的氧化脱除率由改性前的70.5%提高到93.9%。最佳改性条件为:TPAOH的浓度0.4mol/l,改性温度413K,改性时间24h。The micron-scale TS-1 was modified by tetrapropylammonium hydroxide（TPAOH）. The modified TS-1 was used as the catalyst in oxidative desulfurization of 2-methylthiophene from model fuel with H2O2 as oxidant. The samples before and after modification were characterized by XRD, UV-vis, N2 physical adsorption/desorption and TEM techniques. The effects of modification conditions on the performance of the modified TS-1 in 2-methylthiophene removal were investigated, including the concentration of TPAOH, the modification temperature and the modification time. It is shown that the modified sample possessed the typical MFI structure. After modification, the content of framework titanium as well as the extra-framework titanium in TS-1 decreased. However, the modified sample had larger surface area and pore volume than the original sample. In addition, some larger pores of about 1.4 nm and 40-60 nm were found in the modified TS-1 sample, which might be responsible for the improvement of catalytic performance of TS-1. The modified sample exhibited excellent activity in oxidative removal of 2-methylthiophene, with the removal rate of 93.9%, much higher than that of original sample （70.5%）. The optimal modification conditions were as follows： the TPAOH concentration of 0.4 mol/1, the temperature of 413 K, the time of 24 h.

关 键 词：氧化脱硫 TS-1 2-甲基噻吩 过氧化氢 TPAOH 改性 

分 类 号：O643[理学—物理化学]