MOFs限域多酸团簇的合成及其成型化研究进展

doi:10.16085/j.issn.1000-6613.2023-2186

化工进展 ›› 2024, Vol. 43 ›› Issue (12): 6968-6982.DOI: 10.16085/j.issn.1000-6613.2023-2186

• 资源与环境化工 • 上一篇

MOFs限域多酸团簇的合成及其成型化研究进展

薛丽丽¹(), 吴嘉琪¹, 李壮壮¹, 李斯文¹(), 王伟¹, 赵建社²

^1.长安大学水利与环境学院旱区地下水文与生态效应教育部重点实验室，水利部旱区生态水文与水安全重点实验室，陕西西安 710064
^2.西北大学化学与材料科学学院，陕西西安 710069

收稿日期:2023-12-12 修回日期:2024-04-07 出版日期:2024-12-15 发布日期:2025-01-11
通讯作者: 李斯文
作者简介:薛丽丽（2001—），女，硕士研究生，研究方向为氧化脱硫。E-mail：xuelili@chd.edu.cn。
基金资助:
长安大学研究生科学创新实践项目(300103723056)

Research progress in the synthesis and molding of MOFs confined POM

XUE Lili¹(), WU Jiaqi¹, LI Zhuangzhuang¹, LI Siwen¹(), WANG Wei¹, ZHAO Jianshe²

^1.School of Water and Environment, Key Laboratory of Subsurface Hydrology and Ecological Effect in Arid Region of the Ministry of Education, Key Laboratory of Eco-hydrology and Water Security in Arid and Semi-arid Regions of Ministry of Water Resources, Chang’an University, Xi’an 710064, Shaanxi, China
^2.College of Chemistry & Material Science, Northwest University, Xi’an 710069, Shaanxi, China

Received:2023-12-12 Revised:2024-04-07 Online:2024-12-15 Published:2025-01-11
Contact: LI Siwen

摘要/Abstract

摘要：

多金属氧酸盐（POM），简称多酸，是一种具有优异性能的催化剂，但是其通常易溶于有机溶剂，且比表面积较小，导致回收和循环困难。同时，金属有机框架（MOFs）是一种比表面积大、孔隙率高、孔道结构丰富且孔径可调的多孔负载材料。本文从多孔MOFs材料出发，综述了如何促使POM进入MOFs孔隙中，构建得到一类MOFs限域的POM材料（POM@MOF），阐明该类催化材料不仅可以发挥POM高效催化的性能，同时可以有效利用MOFs多孔性能，并对其在氧化脱硫领域的研究现状进行了梳理。然而，即使传统的粉末催化剂具有较优的催化性能，但是不易回收、影响循环使用等问题限制了其在实际生产中的应用。因此，将POM@MOF通过成型纤维固载、静电纺丝等方法进行成型化处理是一条行之有效的方式。最后，本文对成型化POM@MOF在氧化脱硫领域的应用进行了展望，并提出了POM@MOF成型化是未来脱硫领域应用的重要方向之一。

关键词: 催化剂, 金属有机框架, 多金属氧酸盐, 氧化, 再生

Abstract:

Polyoxometalate (POM) is a kind of catalyst with excellent properties, but it is usually soluble in organic solvents and has a small specific surface area, which makes recovery and recycling difficult. Meanwhile, metal-organic framework (MOFs) is a porous loading material with a large specific surface area, high porosity, rich pore structure, and adjustable pore size. Starting from porous MOFs materials, this article reviewed how to promote POM to enter the pores of MOFs, constructing a type of MOFs confined POM material (POM@MOF). It clarified that this type of catalytic material could not only exert the efficient catalytic performance of POM, but also effectively utilize the porous properties of MOFs. The current research status in the field of oxidative desulfurization was also summarized. However, even though traditional powder catalysts had superior catalytic performance, their application in practical production was limited by issues such as difficulty in recovery and impact on recycling. Therefore, it was an effective way to shape and treat POM@MOF through methods such as forming fiber fixation and electrospinning. Finally, this article provided an outlook for the application of POM@MOF in the field of oxidative desulfurization, and proposed that the formation of POM@MOF was one of the important directions for future desulfurization applications.

Key words: catalyst, metal-organic framework, polyoxometalates, oxidation, regeneration

中图分类号:

X511

薛丽丽, 吴嘉琪, 李壮壮, 李斯文, 王伟, 赵建社. MOFs限域多酸团簇的合成及其成型化研究进展[J]. 化工进展, 2024, 43(12): 6968-6982.

XUE Lili, WU Jiaqi, LI Zhuangzhuang, LI Siwen, WANG Wei, ZHAO Jianshe. Research progress in the synthesis and molding of MOFs confined POM[J]. Chemical Industry and Engineering Progress, 2024, 43(12): 6968-6982.

图/表 10

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MOFs种类	结构	代表	孔径/Å	BET比表面积/m²·g^-1
网状金属-有机骨架材料IRMOF^[25-27]	[Zn₄O]⁶⁺四面体为中心连接芳香羧酸有机配体	MOF-5 （IRMOF-1）	15	630~2900
类沸石咪唑酯骨架材料ZIF^[28-29]	过渡金属离子（Zn²⁺/Co²⁺）和咪唑类配体的Ｎ原子结合形成，具有沸石拓扑结构	ZIF-8	11	1500
莱瓦西尔骨架材料 MIL^[30-33]	过渡金属元素与二元羧酸配体合成或者三、四价金属离子（V、Fe、Cr、Al等）与对苯二甲酸等有机配体合成	MIL-101(Fe)	23~27	2800
孔-通道式骨架材料PCN^[34-35]	孔笼-孔道状拓扑结构	HKUST-1	8	1000~1458
UiO^[36-37]	由锆氧簇与羧酸类配体（如对苯二甲酸、均苯三甲酸等）链接形成，具有立体网状结构	UiO-66	8、11	1000

MOFs种类	结构	代表	孔径/Å	BET比表面积/m²·g^-1
网状金属-有机骨架材料IRMOF^[25-27]	[Zn₄O]⁶⁺四面体为中心连接芳香羧酸有机配体	MOF-5 （IRMOF-1）	15	630~2900
类沸石咪唑酯骨架材料ZIF^[28-29]	过渡金属离子（Zn²⁺/Co²⁺）和咪唑类配体的Ｎ原子结合形成，具有沸石拓扑结构	ZIF-8	11	1500
莱瓦西尔骨架材料 MIL^[30-33]	过渡金属元素与二元羧酸配体合成或者三、四价金属离子（V、Fe、Cr、Al等）与对苯二甲酸等有机配体合成	MIL-101(Fe)	23~27	2800
孔-通道式骨架材料PCN^[34-35]	孔笼-孔道状拓扑结构	HKUST-1	8	1000~1458
UiO^[36-37]	由锆氧簇与羧酸类配体（如对苯二甲酸、均苯三甲酸等）链接形成，具有立体网状结构	UiO-66	8、11	1000

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MOFs限域多酸团簇的合成及其成型化研究进展

Research progress in the synthesis and molding of MOFs confined POM

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