Diesel fuel desulfurization with hydrogen peroxide promoted by formic acid and catalyzed by activated carbon

被引:184
作者
Yu, GX [1 ]
Lu, SX [1 ]
Chen, H [1 ]
Zhu, ZN [1 ]
机构
[1] E China Univ Sci & Technol, UNILAB Res Ctr Chem React Engn, Shanghai 200237, Peoples R China
关键词
activated carbon; surface treatment; adsorption properties; catalytic properties; porosity;
D O I
10.1016/j.carbon.2005.04.008
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Desulfurization of diesel fuels with hydrogen peroxide was studied using activated carbons as the catalysts. Adsorption and catalytic properties of activated carbons for dibenzothiophene (DBT) were investigated. The higher the adsorption capacity of the carbons is, the better the catalytic performance in the oxidation of DBT is. The effect of aqueous pH on the catalytic activities of the activated carbons was also investigated. Oxidation of DBT is enhanced when the aqueous pH is less than 2, and addition of formic acid can promote the oxidation. The effect of carbon surface chemistry on DBT adsorption and catalytic activity was also investigated. Adsorption of DBT shows a strong dependence on carboxylic group content. The oxidative removal of DBT increases as the surface carbonyl group content increases. Oxidative desulfurization of a commercial diesel fuel (sulfur content, 800 wt. ppm) with hydrogen peroxide was investigated in the presence of activated carbon and formic acid. Much lower residual sulfur content (142 wt. ppm) was found in the oxidized oil after the oxidation by using the hydrogen peroxide-activated carbon formic acid system, compared with a hydrogen peroxide-formic acid system. The resulting oil contained 16 wt. ppm of sulfur after activated carbon adsorption without any negative effects in the fuel quality, and 98% of sulfur could be removed from the diesel oil with 96.5% of oil recovery. Activated carbon has high catalytic activity and can be repeatedly used following simple water washing, with little change in catalytic performance after three regeneration cycles. (C) 2005 Elsevier Ltd. All rights reserved.
引用
收藏
页码:2285 / 2294
页数:10
相关论文
共 33 条
[1]   DESULFURIZATION OF ORGANIC SULFUR-COMPOUNDS BY SELECTIVE OXIDATION .1. REGENERABLE AND NONREGENERABLE OXYGEN CARRIERS [J].
ATTAR, A ;
CORCORAN, WH .
INDUSTRIAL & ENGINEERING CHEMISTRY PRODUCT RESEARCH AND DEVELOPMENT, 1978, 17 (02) :102-109
[2]   Science and technology of novel processes for deep desulfurization of oil refinery streams: A review [J].
Babich, IV ;
Moulijn, JA .
FUEL, 2003, 82 (06) :607-631
[3]   SOME ASPECTS OF THE SURFACE-CHEMISTRY OF CARBON-BLACKS AND OTHER CARBONS [J].
BOEHM, HP .
CARBON, 1994, 32 (05) :759-769
[4]   Oxidation of high sulphur coal. Part 2. Desulphurisation of organic sulphur by hydrogen peroxide in presence of metal ions [J].
Borah, D ;
Baruah, MK ;
Haque, I .
FUEL, 2001, 80 (10) :1475-1488
[5]   Oxidative desulphurisation of oils via hydrogen peroxide and heteropolyanion catalysis [J].
Collins, FM ;
Lucy, AR ;
Sharp, C .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 1997, 117 (1-3) :397-403
[6]  
DOLBEAR GE, 2000, PREPR AM CHEM SOC DI, V45, P375
[7]   CHEMICAL REACTIVITY OF CARBONS [J].
DONNET, JB .
CARBON, 1968, 6 (02) :161-&
[8]  
ELMER CL, 1940, J PHYS CHEM, V44, P70
[9]   Modification of the surface chemistry of activated carbons [J].
Figueiredo, JL ;
Pereira, MFR ;
Freitas, MMA ;
Orfao, JJM .
CARBON, 1999, 37 (09) :1379-1389
[10]   The sorption of iodine and catalytic decomposition of hydrogen peroxide solution, by Norit charcoals a comparison of the sorption and catalytic activities [J].
Firth, JB ;
Watson, FS .
JOURNAL OF PHYSICAL CHEMISTRY, 1925, 29 :987-994