Self-assembly of Dawson-type H6P2W18O62@[Cu6O(TZI)3(H2O)6]4 for high-performance aerobic oxidation desulfurization of fuel†

IF 3.5 3区 化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Dalton Transactions Pub Date : 2024-07-03 DOI:10.1039/D4DT01568A
Wenjia Qu, Pengpeng Wei, Jingfang Li, Liye Liang, Liqiang Ma and Guangming Li
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Abstract

Because global sulfur emission has escalated, the development of high-efficiency deep desulfurization techniques has become imperative. Herein, to design a high-activity heterogeneous catalyst for the aerobic oxidation desulfurization (AODS) of fuel, Dawson-type polyoxometalate (H6P2W18O62 abbreviated as D-P2W18), characterized by its high activity and strong oxidative capacity, was applied to react with CuCl2·2H2O and H3TZI via a one-pot hydrothermal method. Consequently, blue crystalline H6P2W18O62@[Cu6O(TZI)3(H2O)6]4 (abbreviated as D-P2W18@rht-MOF-1; rht-MOF-1 = [Cu6O(TZI)3(H2O)6]4·nH2O) was afforded. X-ray diffraction analysis indicated that D-P2W18 was successfully encapsulated in two different cages of rht-MOF-1, which is distinct from the crystal structure of Keggin-type POMs@rht-MOF-1. It represents the first crystal structure of Dawson-type POMs@rht-MOF-1. When D-P2W18@rht-MOF-1 was employed as a catalyst for AODS under ambient oxygen pressure with the assistance of surfactant dioctadecyl dimethyl ammonium chloride (DODMAC), it demonstrated remarkable catalytic capability and recyclability for both model fuel and commercial diesel. Further, the AODS reaction mechanism, identified as a free radical oxidation–reduction process, was verified by way of radical quenching experiments, EPR and XPS analysis. This approach offers a feasible route for the synthesis of new Dawson-type POMs@MOFs of heterogeneous catalysts for highly active AODS of fuel.

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自组装 Dawson-type H6P2W18O62@[Cu6O(TZI)3(H2O)6]4,实现燃料的高效有氧氧化脱硫
随着全球硫排放标准的不断提高,开发高效的深度脱硫技术势在必行。为了设计一种用于燃料有氧氧化脱硫(AODS)的高活性异相催化剂,研究人员采用一锅水热法将具有高活性和强氧化能力的道森型多氧金属酸盐(H6P2W18O62,简称 D-P2W18)与 CuCl2-2H2O 和 H3TZI 反应,得到了蓝色晶体 H6P2W18O62@[Cu6O(TZI)]。结果得到了蓝色晶体 H6P2W18O62@[Cu6O(TZI)3(H2O)6]4(简称 D-P2W18@rht-MOF-1;rht-MOF-1 = [Cu6O(TZI)3(H2O)6]4-nH2O)。X 射线衍射分析表明,D-P2W18 成功地被封装在 rht-MOF-1 的两个不同笼子中,这与 Keggin 型 POMs@rht-MOF-1 的晶体结构截然不同。它代表了 Dawson-type POMs@rht-MOF-1 的首个晶体结构。在表面活性剂双十八烷基二甲基氯化铵(DODMAC)的辅助下,D-P2W18@rht-MOF-1 在环境氧压下用作 AODS 催化剂,对模型燃料和商用柴油均表现出显著的催化能力和可回收性。此外,还通过自由基淬灭实验、EPR 和 XPS 分析验证了 AODS 的反应机理,即自由基氧化还原过程。这种方法为合成新型 Dawson-type POMs@MOFs 异相催化剂提供了一条可行的路线,可用于高活性燃料 AODS。
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来源期刊
Dalton Transactions
Dalton Transactions 化学-无机化学与核化学
CiteScore
6.60
自引率
7.50%
发文量
1832
审稿时长
1.5 months
期刊介绍: Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.
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