Well-construction of hollow-pocket shaped Zn-based metal-organic framework for boosting the capture ability towards thiophene sulfur

IF 4.3 2区 材料科学 Q2 ENGINEERING, CHEMICAL Particuology Pub Date : 2025-04-01 Epub Date: 2025-03-05 DOI:10.1016/j.partic.2025.02.017
Qiaolan Yu , Tingting Zhan , Zhouheng Xia , Gaojie Lu , Na Ma , Wei Dai
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Abstract

Conventional metal-organic frameworks (MOFs) have potential applications in adsorption desulfurization due to their open metal sites, structural diversity, and high specific surface area. However, the narrow internal pores limit the adsorption and diffusion of thiophene sulfur molecules (TSM). Therefore, we constructed a novel hollow-type Zn-BTC (HZB) adsorbent by a self-assembled hydrothermal method without using dopant templating agents. The presence of a large internal cavity can be seen by SEM. The results of batch tests showed that the hollow structure Zn-BTC has higher sulfur absorption capacity and faster diffusion rate. The adsorption isotherms were in good agreement with both Freundlich and Dubinin-Radushkevich (D-R) models, suggesting multilayer adsorption combined with pore-filling effect. The maximum adsorption capacity of the TSMs could reach 80% within 30 min, which enabled rapid adsorption in accordance with the pseudo-second-order kinetic model. The adsorption mechanism involves pore filling, ligand effect, and π-π attraction. In addition, HZB-3 maintained good adsorption capacity after the fifth cycle, showing good reusability and stability. This work provides a new strategy for TMS capture using hollow MOF.

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为提高对噻吩硫的捕获能力,精心构建了空心袋形锌基金属有机骨架
传统的金属有机骨架具有开放的金属位点、结构多样性和高比表面积等优点,在吸附脱硫方面具有潜在的应用前景。然而,内部狭窄的孔隙限制了噻吩硫分子(TSM)的吸附和扩散。因此,我们在不使用掺杂模板剂的情况下,采用自组装水热法制备了一种新型空心型Zn-BTC (HZB)吸附剂。扫描电镜可以看到一个大的内腔的存在。批量试验结果表明,空心结构Zn-BTC具有较高的吸硫能力和较快的扩散速率。吸附等温线与Freundlich和Dubinin-Radushkevich (D-R)模型吻合较好,表明多层吸附结合了孔隙填充效应。TSMs的最大吸附容量在30 min内可达到80%,符合准二级吸附动力学模型。吸附机理包括孔填充、配体效应和π-π吸引。此外,HZB-3在第五次循环后仍保持良好的吸附能力,表现出良好的可重复使用性和稳定性。这项工作为利用空心MOF捕获TMS提供了一种新的策略。
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来源期刊
Particuology
Particuology 工程技术-材料科学:综合
CiteScore
6.70
自引率
2.90%
发文量
1730
审稿时长
32 days
期刊介绍: The word ‘particuology’ was coined to parallel the discipline for the science and technology of particles. Particuology is an interdisciplinary journal that publishes frontier research articles and critical reviews on the discovery, formulation and engineering of particulate materials, processes and systems. It especially welcomes contributions utilising advanced theoretical, modelling and measurement methods to enable the discovery and creation of new particulate materials, and the manufacturing of functional particulate-based products, such as sensors. Papers are handled by Thematic Editors who oversee contributions from specific subject fields. These fields are classified into: Particle Synthesis and Modification; Particle Characterization and Measurement; Granular Systems and Bulk Solids Technology; Fluidization and Particle-Fluid Systems; Aerosols; and Applications of Particle Technology. Key topics concerning the creation and processing of particulates include: -Modelling and simulation of particle formation, collective behaviour of particles and systems for particle production over a broad spectrum of length scales -Mining of experimental data for particle synthesis and surface properties to facilitate the creation of new materials and processes -Particle design and preparation including controlled response and sensing functionalities in formation, delivery systems and biological systems, etc. -Experimental and computational methods for visualization and analysis of particulate system. These topics are broadly relevant to the production of materials, pharmaceuticals and food, and to the conversion of energy resources to fuels and protection of the environment.
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