磷钨酸∕SBA-15催化氧化-萃取柴油脱硫.pdf

化工.进展
CIIEMICAL NDUSTRY AND ENGNEERING PROGRESS
2016年第35卷第9期
reuser
研究开发
磷钨酸SBA-15催化氧化-萃取柴油脱硫
李瑞丽,昌本震,蒋善良,李晶品
中国石油大学(北京)重质油国家重点实验室,北京102249)
摘要:以自制的SBA-15为載体,磷钨酸为活性组分,用过量浸渍法制备了 AIPW/SBA-15催化剂,并采用SEM
BHT和(G-HDIA对催化剂进行表征分析。H2O)2为氧化剂,十六烷基三甲基澳化铵(CIAB)为相转移剂,以二
苯并吩(DBT)的模型化合物(DBT为溶质、正辛烷为溶剤)进行氧化脱除为探针反应,考察了磷钨酸负载
量和 IIPW/SBA-15的焙娆温度对催化剂活性的影响,同时考察了氧化-萃取工艺条件对真实柴油脱硫效果的影响
实验结果表明,礫钨酸最住负戟量为30%, HPW/SBA-15在250℃焙烧处理时活性最高;在m(H2O)2):n(S)6、
HPW,SBA-15用量为2.5%(基于柴油质量)、CIAB用蛩为0.4%(基于柴油质量)、萃取级数为4、温度60℃反
应15h的条件下,柴油硫含量从1317mgL降到39mgL,脱硫卒达到97.09%、收率不低于85.0%。气相色谱结
果显示,该催化氧化脱硫体系容易脱除柴油中加氢难以脱除的二苯并嘿吩及其衍生物
关键词:SBA-15;载体;磷钨酸;催化剂;催化氧化;萃取;柴油;脱硫
中图分类号:TH626
文献标志码:A
文章编号:1000-6613(2016)09-2790-06
DOI:10.160851.1ssn.1000-6613.2016.09.022
Diesel desulfurization by phosphotungstic acid/sba-15 catalytic
oxidation-extraction
LI Ruili, L1 Benzhen, LANG Shanliang, LI Jingiing
State Key Laboratory of Heavy Oil Processing, China University of Petroleum-beijing, Beijing 102249, China)
Abstract: A series of HPW/SBA-15 were prepared by supersaturated impre nation method with
phosphotungstic acid loaded on SBA-15. The catalysts wcre characterized by means of BET, SEM and
TG-DTA. The effects of HPW loading amount and calcination temperature on the desulfurization were
nvestigated by studying the DBT desulfurization performance on the HPW/SBA-15 with H202 as
oxidation and CTAB as phasc transfer catalyst. Mcanwhilc, thc cffccts of diffcrcnt oxidation-cxtraction
conditions on diesel desulfuriation were investigaled. The results showed that the best mass
percentage of FPW was 30% and HPW/SBA-15 showed the highest activity al 250C. The sulful
content in the diesel oil decreased from 1317mg/L to 39mg/L and the sulfur removal rate reached
97.0 under the best condition of n( H202): n(S)=6, the mass percentage of HPW/SBA-15 of 2.5%
that of CTAB of 0.4%(both bascd on th dicscl oil), cxtraction stagc of 4, rcaction tcmpcralurc of60 C
and reaction time of I 5h. According to GC analysis, the HPW/SBA-15 catalytic oxidation-extraction
method could easily remove dibenzothiophene and its derivatives, which were quite inert in diesel
during its hydrodesulfurization
Key words: SBA-15; support; phosphotungstic acid; catalyst; catalytic oxidation; cxtraction: dicscl
desulfurization
随着坏保意识的增强,世界主要困家均制定了
收稿日期:2015-11-09:修改稿日期:2016-03-23
第一作者及联系人:李瑞丽(1965一),女,倾土,副研究员,从事清
日趋严格的硫含量标准。为了顺应世界标准,缩
清油品生产的教学与研究工作。T- mail IT4806a163,com