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功能化 Y-SBA-15 固载多金属氧酸盐催化剂上的超快柴油燃料氧化脱硫。

Ultrafast oxidative desulfurization of diesel fuel catalyzed by a polyoxometalate-based catalyst immobilized on functionalized Y-SBA-15.

机构信息

Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Key Laboratory of Green Chemical Process of Ministry of Education, Hubei Key Laboratory of Novel Chemical Reactor and Green Chemical Technology, Wuhan Institute of Technology, Wuhan 430073, P. R. China.

School of Environment and Natural Resources, Renmin University of China, Beijing 100872, P. R. China.

出版信息

Dalton Trans. 2022 Jun 27;51(25):9864-9877. doi: 10.1039/d2dt00911k.

Abstract

Y-SBA-15 was synthesized by doping yttrium (Y) into SBA-15 using a solvent-free solid-state grinding method, and 1-butyl-3-methylimidazolium phosphomolybdic salt ([Bmim]PMoO, abbreviated as [Bmim]PMoO) was also synthesized. [Bmim]PMoO/Y-SBA-15 was prepared and used for oxidative desulfurization (ODS). The physicochemical characteristics of the catalyst have been characterized by FT-IR, XRD, N adsorption-desorption, FESEM, TEM, XPS, contact angle testing, EPR, . A lipophilic surface is beneficial for making the catalyst well disperse in an oil phase, and a hydrophilic core can help to store aqueous oxidants. Therefore, the amphiphilic catalyst 25[Bmim]PMoO/10Y-SBA-15 exhibited high catalytic activity in dibenzothiophene (DBT) ODS, and sulfur compounds can be removed completely within 40 min under the following conditions: = 10 mL, = 0.1 g,  :  = 25%, and O/S = 4 (molar ratio). In addition, the concentration of aromatics exerted little effect on the DBT ODS. Sulfur compounds in real diesel might be reduced to 8 μg g. The hydroxyl radical ˙OH and superoxide radical ˙O play crucial roles in the ODS reaction, and the ODS reaction mechanism was also proposed.

摘要

Y-SBA-15 是通过无溶剂固态研磨法将钇(Y)掺杂到 SBA-15 中合成的,同时还合成了 1-丁基-3-甲基咪唑磷钼酸盐([Bmim]PMoO,简称[Bmim]PMoO)。[Bmim]PMoO/Y-SBA-15 被制备并用于氧化脱硫(ODS)。通过 FT-IR、XRD、N 吸附-脱附、FESEM、TEM、XPS、接触角测试、EPR 等对催化剂的物理化学性质进行了表征。疏水性表面有利于催化剂在油相中的良好分散,而亲水性核有助于储存水相氧化剂。因此,具有两亲性的催化剂 25[Bmim]PMoO/10Y-SBA-15 在二苯并噻吩(DBT)ODS 中表现出很高的催化活性,在以下条件下 40 分钟内可以完全去除硫化合物:= 10 mL,= 0.1 g,= 25%,O/S = 4(摩尔比)。此外,芳烃浓度对 DBT ODS 的影响很小。实际柴油中的硫化合物可能会减少到 8μg g。羟基自由基˙OH 和超氧自由基˙O 在 ODS 反应中起着至关重要的作用,同时还提出了 ODS 反应机制。

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