催化氧化-萃取集成燃油脱硫工艺研究
发布时间：2018-09-06 08:43
【摘要】：本文主要研究了利用催化氧化萃取集成体系,非均相催化氧化脱除燃油中硫化物。使用等体积浸渍法制备的Mo/y-Al2O3催化剂表现出优良的催化活性。通过对催化剂进行了XRD、H2-TPR和N2吸附-脱附表征,表明催化剂具有介孔结构,Al2(MoO4)3是催化氧化的主要活性组分。考察了乙腈、甲醇、N,N-二甲基甲酰胺、N-甲基吡咯烷酮和水作为萃取剂对催化氧化萃取集成脱硫体系的影响,乙腈和甲醇表现出协同脱硫作用和优良的溶剂特性。以Mo(16wt%)/γ-Al2O3作为催化剂,在n(H2O2)/n(S)=2.3、反应温度60℃、v(模拟油)/v(乙腈)=3/1、催化剂用量0.2 g的条件下,苯并噻吩、二苯并噻吩和4,6-二甲基二苯并噻吩在40min内可以被完全氧化脱除。反应过程中由于萃取剂的存在减弱了催化剂对产物砜类的吸附,催化剂寿命得到显著延长。反应过程分为两步,首先含硫化合物被萃取至萃取剂相中,然后在催化剂的催化作用下被H202氧化为砜类物质,其中液液萃取过程速率相对较快,氧化反应过程被认为是整个反应体系的速率控制步骤。通过对动力学模型进行假设,反应体系包括液液传质、液固传质和氧化反应三个过程,通过对动力学参数进行计算分析认为,反应符合一级反应动力学。以Mo/γ-Al2O3作为催化剂对噻吩的催化氧化效果较低,所以针对噻吩,采用非均相类Fenton氧化体系,制备了XO-Fe2O3/y-Al2O3(X为第二种金属元素)作为催化剂,以水作为萃取剂,研究了非均相类Fenton体系对噻吩的催化氧化效果。对催化剂进行了XRD、SEM和N2吸附-脱附表征。Fe2O3/γ-Al2O3具有一定催化H202氧化噻吩的活性,说明非均相类Fenton试剂可以催化H202产生OH。Fe2O3/y-Al2O3掺杂少量其它金属可以改变其催化活性,其中以加入Cu元素后催化活性最高,说明Cu元素起到了催化剂助剂的作用,催化剂呈现明显的介孔性质。Cu和Fe的负载量分别为0.6%和15%的CuO-Fe2O3/y-Al2O3的催化活性最高。在反应温度60℃、v(模拟油)/v(水)=3/1、催化剂加入量0.2 g,n(H2O2)/n(Th)=7.40和反应时间为120 mmin的条件下,噻吩脱除率达到95%以上,同样达到超深度脱硫的效果。
[Abstract]:In this paper, heterogeneous catalytic oxidation is used to remove sulfides from fuel oil by catalytic oxidation extraction system. The Mo/y-Al2O3 catalyst prepared by equal volume impregnation method showed excellent catalytic activity. The adsorption-desorption schedule of XRD,H2-TPR and N2 showed that Al _ 2 (MoO4) _ 3 with mesoporous structure was the main active component in catalytic oxidation. The effects of acetonitrile, methanol N-dimethylformamide N-methylpyrrolidone and water as extractant on catalytic oxidative extraction integrated desulfurization system were investigated. Acetonitrile and methanol showed synergistic desulfurization and excellent solvent properties. Using Mo (16wt%) / 纬 -Al _ 2O _ 3 as catalyst, benzothiophene, dibenzothiophene and 4- (6-dimethyldibenzothiophene) can be completely oxidized in 40min under the conditions of n (H2O2) / n (S) 2.3, reaction temperature 60 鈩，
本文编号：2225818
[Abstract]:In this paper, heterogeneous catalytic oxidation is used to remove sulfides from fuel oil by catalytic oxidation extraction system. The Mo/y-Al2O3 catalyst prepared by equal volume impregnation method showed excellent catalytic activity. The adsorption-desorption schedule of XRD,H2-TPR and N2 showed that Al _ 2 (MoO4) _ 3 with mesoporous structure was the main active component in catalytic oxidation. The effects of acetonitrile, methanol N-dimethylformamide N-methylpyrrolidone and water as extractant on catalytic oxidative extraction integrated desulfurization system were investigated. Acetonitrile and methanol showed synergistic desulfurization and excellent solvent properties. Using Mo (16wt%) / 纬 -Al _ 2O _ 3 as catalyst, benzothiophene, dibenzothiophene and 4- (6-dimethyldibenzothiophene) can be completely oxidized in 40min under the conditions of n (H2O2) / n (S) 2.3, reaction temperature 60 鈩，
本文编号：2225818
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