【摘要】：燃油超深度脫硫已經(jīng)成為世界范圍內(nèi)急需的一種環(huán)保技術。作為交通運輸?shù)闹饕剂?柴油和汽油中的硫化物也是導致酸雨、霧霾和腐蝕的主要原因。氧化脫硫就包括了將含硫化合物氧化為相應的砜類物質(zhì)并通過萃取或吸附將其除去的過程。在溫和條件下使用一種新的氧化體系對模型柴油中的含硫化合物(BT,DBT,4,6-DMDBT)進行氧化脫硫。此體系,將Anderson型催化劑(C18H37)2N(CH3)2]3Co(OH)_6Mo_6O_(18)溶解在離子液體[Bpy]BF4中,對模型柴油進行催化氧化脫硫。以氧氣為氧化劑。體系的循環(huán)性能相較于以前的報道有很大提升且對DBT脫除率可達100%。此體系可被循環(huán)五次且活性沒有明顯下降。此外,我們還根據(jù)一種新型的安德森型催化劑進行了催化氧化脫硫研究。新型的Anderson型雜多酸{[(CH3)3N(CH2)2OH]2}[H0.2K0.2Na2.6(H2O)6][IMo6O24]催化劑進是通過低共熔物進行合成的,而后對其進行XRD粉末衍射,傅里葉變換紅外光譜(FTIR),熱重分析使,循環(huán)伏安,ICP-AES表征。將此種雜多酸催化劑溶解到離子液體中對模型柴油進行催化氧化脫硫。這個催化體系包括過作為氧化劑的過氧化氫和1-辛基-3-甲基咪唑四氟硼酸鹽離子液體,其表現(xiàn)出了可以在60℃下60分鐘對DBT達到100%脫除率的高活性。此體系對柴油中幾種常見硫化物脫硫活性順序為DBT4,6-DMDBTBT。此脫硫體系表現(xiàn)出了良好的穩(wěn)定性,其脫硫活性在20次循環(huán)實驗中沒有明顯下降。另外,我們研究了一種以草酸和四丁基氯化銨以1/2摩爾比合成的草酸基低共熔劑催化模型柴油脫除DBT的過程。合成了此種草酸基低共熔劑并用IR,XRD,CV,EPR等方法對其進行表征并探究了其反應機理。作為催化劑和萃取劑,低共熔劑表現(xiàn)出了良好的活性。為了獲得理想的低共熔劑,對低共熔劑的合成方法,氫鍵受體進行了一些列篩選,并確定了其合成的最優(yōu)摩爾比。對反應過程中溫度,氧硫比等影響進行了研究。這種草酸基低共熔劑在60℃條件下,180分鐘可以達到對模型柴油中DBT的98%脫硫率。
[Abstract]:Ultra-deep desulfurization of fuel has become an urgent environmental protection technology all over the world. As the main fuel for transportation, sulfides in diesel and gasoline are also the main causes of acid rain, haze and corrosion. Oxidative desulfurization involves the oxidation of sulfur compounds to corresponding sulfones and their removal by extraction or adsorption. Sulfur compounds (BT,DBT,4,6-DMDBT) in model diesel oil were oxidized by a new oxidation system under mild conditions. In this system, the Anderson catalyst (C18H37) 2N (CH3) 2] 3Co (OH) was dissolved in the ionic liquid [Bpy] BF4, and the model diesel oil was desulfurized by catalytic oxidation. Oxygen is used as oxidant. Compared with previous reports, the cycle performance of the system has been greatly improved and the removal rate of DBT can be up to 100kW. The system can be recirculated five times and the activity does not decrease significantly. In addition, a new type of Anderson catalyst was used to study the catalytic oxidation desulfurization. A new type of Anderson heteropoly acid {[(CH3) 3N (CH2) 2OH] 2} [H0.2K0.2Na2.6 (H2O) 6] [IMo6O24] was synthesized by eutectic material, then was diffracted by XRD powder, characterized by Fourier transform infrared (FTIR) (FTIR), thermogravimetry, cyclic voltammetry ICP-AES. The catalytic oxidation desulfurization of model diesel oil was carried out by dissolving the heteropoly acid catalyst into ionic liquids. The catalytic system consists of hydrogen peroxide and 1-octyl -3-methylimidazolium tetrafluoroborate ionic liquids, which exhibit a high activity of 100% removal of DBT at 60 鈩，

本文編號：2261349