Liu Liyan, Zhang Yu, Tan Wei
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.
School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.
Ultrason Sonochem. 2014 May;21(3):970-4. doi: 10.1016/j.ultsonch.2013.10.028. Epub 2013 Nov 8.
Phosphotungstic acid (HPW) supported on activated carbon (AC) was applied to catalyze deep oxidation desulfurization of fuel oil with the assist of ultrasound. The sulfur-conversion rate was evaluated by measuring the concentration of dibenzothiophene (DBT) in n-octane before and after the oxidation. Supporting HPW on AC has been verified to play a positive role in UAOD process by a series of contrast tests, where only HPW, AC or a mixture of free HPW and AC was used. The influences of catalyst dose, ultrasound power, reaction temperature, H2O2:oil volume ratio and the reuse of catalyst on the catalytic oxidation desulfurization kinetics were investigated. The DBT conversion rate of the reaction catalyzed by supported HPW under ultrasound irradiation was higher than the summation of the reactions with HPW only and AC only as catalyst. With the increase of loading amount of HPW on AC, ultrasound power, H2O2:oil volume ratio and reaction temperature, the catalytic oxidation reactivity of DBT would be enhanced. The optimum loading amount of HPW was 10%, exceed which DBT conversion would no longer increase obviously. DBT could be completely converted under the optimized conditions (volume ratio of H2O2 to model oil: 1:10, mass ratio of the supported HPW to model oil: 1.25%, temperature: 70°C) after 9 min of ultrasound irradiation.
将负载在活性炭(AC)上的磷钨酸(HPW)用于在超声辅助下催化燃油深度氧化脱硫。通过测量氧化前后正辛烷中二苯并噻吩(DBT)的浓度来评估硫转化率。通过一系列对比试验验证了在AC上负载HPW在超声辅助氧化脱硫(UAOD)过程中发挥了积极作用,在这些试验中仅使用了HPW、AC或游离HPW与AC的混合物。研究了催化剂用量、超声功率、反应温度、H2O2与油的体积比以及催化剂的重复使用对催化氧化脱硫动力学的影响。在超声辐照下,负载HPW催化的反应中DBT转化率高于仅以HPW和仅以AC为催化剂的反应之和。随着HPW在AC上负载量、超声功率、H2O2与油的体积比以及反应温度的增加,DBT的催化氧化反应活性增强。HPW的最佳负载量为10%,超过此值DBT转化率不再明显增加。在优化条件下(H2O2与模拟油的体积比为1:10,负载HPW与模拟油的质量比为1.25%,温度为70°C),超声辐照9分钟后DBT可完全转化。