大学化学 >> 2022, Vol. 37 >> Issue (5): 2110079.doi: 10.3866/PKU.DXHX202110079

所属专题： 第2届全国大学生化学实验创新设计竞赛

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多酸基共价有机骨架材料的合成与氧化脱硫性能研究在实验教学中的设计与探究

刘世超, 李雅宁, 詹宇璇, 王晓红(), 邹小勤()   

  • 收稿日期:2021-10-25 录用日期:2021-11-04 发布日期:2022-03-18
  • 通讯作者: 王晓红,邹小勤 E-mail:wangxh665@nenu.edu.cn;zouxq100@nenu.edu.cn
  • 作者简介:邹小勤, Email: zouxq100@nenu.edu.cn
    王晓红, Email: wangxh665@nenu.edu.cn
  • 基金资助:
    国家自然科学基金(51978134)

Design and Exploration of Synthesis and Oxidative Desulfurization Study of Polyoxometalate-Based Covalent Organic Framework in Experimental Teaching

Shichao Liu, Yaning Li, Yuxuan Zhan, Xiaohong Wang(), Xiaoqin Zou()   

  • Received:2021-10-25 Accepted:2021-11-04 Published:2022-03-18
  • Contact: Xiaohong Wang,Xiaoqin Zou E-mail:wangxh665@nenu.edu.cn;zouxq100@nenu.edu.cn

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摘要：

化石燃料燃烧带来的硫排放将导致酸雨的产生，因而实现燃油深度脱硫显得至关重要。多酸(POM)基共价有机骨架材料具有氧化还原性、可调的亲疏水性、可循环再生等特点，被认为是燃油氧化脱硫的一种优异催化材料。本实验在科研成果的基础上创新设计了一个综合实验。通过离子交换法将强氧化型多酸分子(NH4)5H6PMo4V8O40 (简写为PMo4V8)引入共价有机骨架(COF)，合成了一种多酸基共价有机骨架材料(POM@EB-COF，EB代表溴化乙啶)。利用X射线衍射、红外光谱、元素分析等表征手段对材料结构进行解析。以含有二苯并噻吩的十氢萘作为模型燃油，体系中通入氧气，在PMo4V8@EB-COF固体材料表面进行二苯并噻吩的氧化反应，考察其氧化脱硫性能。研究结果表明，以PMo4V8@EB-COF作为氧化脱硫催化剂，反应温度为100 ℃，反应时间2.5 h，二苯并噻吩(DBT)的转化率达96.6%，DBT氧化产物砜的选择性达100%，PMo4V8@EB-COF展现出优异的催化性能。本实验涉及多个化学二级学科的知识要点，普及了合成化学与绿色化学的理念，也适用于模块化实验教学以满足不同教学要求，提高了学生的创新意识和综合能力。

关键词: 多酸, 共价有机骨架, 氧化脱硫, 新创实验

Abstract:

Sulfur emission from fossil fuel combustion can lead to acid rain; thus, it is essential to reduce the sulfur content of fuel through deep desulfurization. The polyoxometalate (POM)-based covalent organic framework (COF) is considered an excellent catalytic material because it exhibits excellent redox activity, adjustable hydrophilicity, and good recyclability. The successful encapsulation of vanadium-containing POM ((NH4)5H6PMo4V8O40, PMo4V8) into EB-COF (EB represents ethidium bromide) is achieved via ion exchange, and a new composite of PMo4V8@EB-COF is produced. The composite structure is determined through X-ray diffraction analysis, infrared spectroscopy, and elemental analysis. The oxidative desulfurization potential of PMo4V8@EB-COF is studied using dibenzothiophene as a model fuel and oxygen as an oxidizer. The catalytic results show that PMo4V8@EB-COF exhibits an excellent desulfurization performance. At 100 ℃, dibenzothiophene (DBT) conversion reaches 96.6% after the reaction for 2.5 h. In this experiment, chemistry knowledge of various subjects as well as concepts of synthesis chemistry and green chemistry are involved. Moreover, this experiment is suitable for modular teaching with individual sections to meet experimental teaching needs. Through this experiment, students can cultivate the spirit of innovation and improve comprehension abilities.

Key words: Polyoxometalates, Covalent organic frameworks, Oxidative desulfurization, Innovation experiment