活性炭负载S2O8 2-/ZrO2催化剂的制备及其催化氧化脱硫性能

采用浸渍沉淀法制备了固体超强酸S2O2-8/ZrO2 AC催化剂,以二苯并噻吩(DBT)的正十二烷溶液为含硫化合物模拟油(硫质量分数为400 μg/g),H2O2为氧化剂,考察催化剂的催化氧化脱硫性能,采用BET、XRD、FT IR和NH3 TPD分析手段对其结构进行了表征。利用所制备的催化剂,考察了反应温度、反应时间、氧化剂用量、催化剂用量和乳化剂Span60用量对脱硫效果的影响。结果表明,当活性组分ZrO2负载量(质量分数)为10%,焙烧温度为650℃,所制备的S2O2-8/ZrO2 AC催化剂的催化氧化脱硫活性最高;其氧化20 mL模拟油的最佳操作条件为反应温度60℃、反应时间60 min、氧化剂/硫摩尔比5、乳化剂Span60用量01g,催化剂用量以每1 mL模拟油添加004 g计。在此条件下,DBT基本全部转化为相应的砜,采用N,N 二甲基甲酰胺(DMF)萃取,DMF/汽油体积比为1/4时,模拟油的脱硫率可以达到976%,回收率为925%,并且催化剂具有较好的稳定性。

Preparation and Performance of Activated Carbon Loaded S2O2-8/ZrO2 Catalyst for Catalytic Oxidative Desulfurization

The S²O^2-₈/ZrO₂-AC solid superacid catalyst was prepared by immersion precipitation method and the oxidative deep desulfurization of model fuel with DBT as model sulfur compound and dodecane as solvent (Sulfur mass fraction of 400 μg/g) was investigated with H2O2as oxidant catalyzed by S2O2-8/ZrO2 AC. The structure of the prepared catalysts was characterized by means of BET, XRD, FTIR and NH3 TPD, respectively. The effects of oxidation temperature, reaction time, the amount of oxidant, the dosage of catalyst and Span60 on the desulfurization performance were also investigated. The results showed that the S2O2-8/ZrO2 AC with ZrO2loading amount of 10% calcined at temperature of 650℃ had a good catalytic activity in oxidative desulfurization. Under the optimal conditions of oxidation temperature 60℃, reaction time 60 min, the molar ratio of the oxidant to sulfur 5, the catalyst dosage 004 g per mL model fuel and the dosage of Span60 01 g, DBT could be substantially converted to sulfone. After oxidation by using the extraction with dimethylformamide (DMF) as extractant and 1/4 volumetric ratio of DMF to model fuel, the sulfur removal efficiency and recovery of model fuel could reach 976% and 925%, respectively. The catalyst could be regenerated as well.