Development of Low Cost Production Process for Sulfur-free Light Hydrocarbon Fuels Using Oxidation-Adsorption

本项目旨在开发一种新型氧化-吸附氧化脱硫工艺。这个过程将在大气压下和低于100℃的温度下进行。制备了一系列氧化催化剂。在流动固定床反应体系中，考察了催化剂对含噻吩(T)、烷基噻吩和苯并噻吩（BT）的刺激性汽油在十氢化萘或异辛烷中的氧化活性。钼基催化剂表现出较高的活性。各种含硫化合物的反应活性如下：BT>2,3,5三甲基噻吩>2-甲基噻吩>2,5-二甲基噻吩>T。此外，兴奋剂汽油中所有含硫化合物的氧化反应均符合一级反应。测定了氧化速率常数和活化能。并对CAT-2催化剂的氧化条件进行了优化。采用氧化催化剂CAT-2和吸附剂AD-1进行氧化吸附脱硫，使兴奋剂汽油的硫含量由15 ppm降至0.10ppm。采用氧化催化剂CAT-1和吸附剂AD-1进行氧化吸附脱硫，使某商品煤油的硫含量由6.0ppm降至0.05ppm以下。

The aim of this project is to develop a novel oxidation desulfurization process using a combination of oxidation-adsorption. This process will operate under atmospheric pressure and at the temperature below 100℃. A series of oxidation catalysts were prepared. The catalytic activities of the catalysts were evaluated in the oxidation of a stimulant gasoline, which contains thiophene(T), alkyl-thiophenes and benzothiophene (BT) in decalin or isooctane, using a flow fixed-bed reaction system. The Mo-based catalysts showed higher activities. The reactivities of various sulfur compounds are as follows : BT>2,3,5Trimethylthiophene>2-methylthiophene>2,5-Dimethylthiphene>T. Further, the oxidation of all the sulfur compounds in the stimulant gasoline was fit using first-order reaction. The oxidation rate constants and the activation energies were estimated. Moreover, oxidation conditions using CAT-2 catalyst were optimized. In the oxidation-adsorption desulfurization using oxidation catalyst CAT-2 and adsorbent AD-1, the sulfur content in a stimulant gasoline decreased from 15 ppm to 0.10ppm. In the oxidation-adsorption desulfurization using oxidation catalyst CAT-1 and adsorbent AD-1, the sulfur content in a commercial kerosene decreased from 6.0ppm to less than 0.05ppm.