Preparation of 30%PMoV2@MOF@mSiO2 (MOF = MIL-101, HKUST-1, UiO-67, ZIF-8) catalysts and their oxidative desulfurization performance

IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2024-10-21 DOI:10.1016/j.mcat.2024.114613

Pushuang Xing , Cong Li , Yixin Chen, Rong-Lan Zhang

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Abstract

PMoV₂ was encapsulated in four MOFs (MIL-101, HKUST-1, UiO-67, ZIF-8) with different cavity sizes and window sizes using a hydrothermal synthesis method. Then, a layer of mesoporous silica was coated on the surface of the MOFs to obtain four designed three-layer encapsulated catalysts 30%PMoV₂@MOF@mSiO₂. The physicochemical properties of the catalysts were characterized through various characterization methods, and the influence of different MOF window sizes of the four catalysts on the removal rate of four thiophene sulfides was investigated. The optimal reaction conditions were also explored for the optimal catalyst. The results indicate that under simulated fuel of 2400 ppm, 30%PMoV₂@UiO-67@mSiO₂ owns the highest catalytic activity. Under optimal conditions, the total removal rate of four thiophene compounds was 91.52 %, and after ten cycles, the efficiency could still reach 86.24 %. This is attributed to the sufficient cavity size of UiO-67, which provides assurance for the loading of PMoV₂ and the large window size, making it possible for the smooth reaction between sulfides and PMoV₂.

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30%PMoV2@MOF@mSiO2 （MOF = MIL-101、HKUST-1、UiO-67、ZIF-8）催化剂的制备及其氧化脱硫性能

采用水热合成法将 PMoV2 封装在四种具有不同空腔尺寸和窗口尺寸的 MOFs（MIL-101、HKUST-1、UiO-67 和 ZIF-8）中。然后，在 MOFs 表面包覆一层介孔二氧化硅，得到四种设计的三层包覆催化剂 30%PMoV2@MOF@mSiO2。通过各种表征方法对催化剂的理化性质进行了表征，并研究了四种催化剂不同的 MOF 窗口尺寸对四种噻吩硫化物去除率的影响。此外，还探讨了最佳催化剂的最佳反应条件。结果表明，在模拟燃料为 2400 ppm 的条件下，30%PMoV2@UiO-67@mSiO2 的催化活性最高。在最佳条件下，四种噻吩化合物的总去除率为 91.52%，经过十次循环后，效率仍可达 86.24%。这归功于 UiO-67 具有足够的空腔尺寸，为 PMoV2 的装填提供了保证，同时其窗口尺寸较大，使硫化物与 PMoV2 的反应得以顺利进行。

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods