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Studies on the Adsorption and Oxidation-Extraction (Adsorption) for Ultra-deep Desulfurization of Diesel Fuels

Author: JiangZongXuan
Tutor: LiCan;HanChongRen
School: Dalian Institute of Chemical Physics
Course: Physical and chemical
Keywords: Activated Carbon Adsorbent Ultra-deep desulfurization Oxidation Catalyst Emulsion
CLC: TE624.5
Type: PhD thesis
Year: 2003
Downloads: 884
Quote: 13
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As more stringent environmental regulations, ultra deep desulfurization of diesel (<15ppm) has become a very urgent and urgent global research. In addition, the source of hydrogen fuel cell system, if the hydrogen from the fuel, then the use of ultra low sulfur or sulfur-free fuel. Although conventional hydrodesulfurization (HDS) can be very effective in removing most of the sulfur-containing, but removal of dibenzothiophene and its derivatives encountered a serious challenge. To hydrogenated diesel oil present in the remaining 200 ~ 500 ppm of sulfur by HDS way down to 15 ppm or less, required at higher temperatures and pressures, lower airspeed, with higher activity catalysts conditions. This is bound to have as many problems: high investment, high operating costs and shorten the life of the catalyst to increase the hydrogen consumption and so on. People in the study currently nonhydrodesulfurization technologies such as adsorption desulfurization, oxidative desulfurization, desulfurization and bio-desulfurization extraction, adsorption and oxidation of an extract of which (adsorption) desulfurization by industry considered a major breakthrough is expected in the near future ultra-deep desulfurization technology. This thesis focuses on the adsorption and oxidation an extraction (adsorption) for ultra deep desulfurization of diesel. In the first part of the work, the system examines the diesel dibenzothiophene adsorption on activated carbon in the modified and the impact of dibenzothiophene on activated carbon adsorption capacity of the main factors; then conducted a systematic characterization of modified activated carbon and characterization and adsorption performance results were correlated. In the second part of the work, by selective catalytic oxidation of the sulfur diesel converted to the corresponding sulfone, then through the extraction (adsorption), can achieve ultra-deep desulfurization of diesel fuel (<0.1 ppm). Dibenzothiophene adsorption on activated carbon in the modified results showed that different modification methods for activated carbon desulfurization rate has a great influence. Activated carbon oxide modification on the desulfurization rate shadow. To the following order: sulfuric acid> concentrated nitric> ammonium peroxodisulfate> Hydrogen peroxide (30%)> potassium permanganate solution. In the modification process of the study, with sulfuric acid (or acid composition other methods) the best modified activated carbon desulfurization, sulfur capacity of activated carbon from the unmodified sulfur 0.0240 g / g of sulfur sorbent increased to 0.0529 g / g adsorbent. Sulfur capacity increase rate is so large, has not been reported. Research on the diesel hydrotreating and sulfur removal rate never modified activated carbon to rise to 23.3% 32.5% sulfuric acid modified activated carbon, indicating sulfuric acid modification is also conducive to the adsorption of sulfur in diesel. Using low-temperature nitrogen adsorption, base titration, infrared spectroscopy, different sizes and polar molecules adsorption experiments investigated activated carbon pore structure, surface properties and dibenzothiophene relationship between adsorption capacity. The results showed that the modified dibenzothiophene on activated carbon adsorption capacity of the activated carbon mainly related to the increase in pore volume and surface of the amount of oxygen-containing groups increased. 4,6 - dimethyl dibenzothiophene and diesel in the selective catalytic oxidation of sulfur compounds results show that metastable emulsion droplets incorporated in the catalyst [(C 18 H 37 ) 2 N (CH 3 ) 2 ] 3 [PW 12 O 40 ] display class homogeneous catalyst performance, with high catalytic activity, capable of mild reaction conditions (30 ℃, atmospheric pressure) for , 4,6 - dimethyl dibenzothiophene and diesel sulfur compounds in complete conversion to the sulfone. Sulfide catalyst selectivity is 100% utilization of hydrogen peroxide over 96%: demulsification by centrifugation after the reaction, the catalyst is recyclable. Generated using the extraction method to selectively remove a sulfone can be the sulfur content of diesel fuel from 500ppm down to less than 0.1 ppm, does not change the nature of the oil. These results have not been reported before. In addition, also inspected the sulfone in the modified activated carbon adsorption, also made some progress.

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CLC: > Industrial Technology > Oil and gas industry > Oil, natural gas processing industry > Petroleum refining > The refining process > Refined treatment
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