金属有机骨架UiO-66的制备及其储氢性能：微波与常规水热法制备的比较

Q3 Energy

燃料化学学报 Pub Date : 2025-04-01 DOI:10.1016/S1872-5813(24)60496-2

Ruiqi Wang , Hengjie Shi , Yanli Sun , Xi Zhang , Caizhu Liu , Yuhua Wu , Jianbo Wu , Hui Zhang , Hongcun Bai

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引用次数: 0

摘要

由于金属有机框架（MOFs）具有结构设计性强、孔隙可调等优点，其高效制备已成为固态储氢领域的重要课题。然而，其高效制备仍面临工艺复杂、周期长、效率低等关键瓶颈。微波辅助合成是一种新兴技术，它利用微波外场来增强多孔材料制备过程中的传质、传热和反应行为，从而有望提高 MOFs 材料的制备效率。该方法被认为是实现 MOFs 材料高效制备的重要发展方向。本研究主要对微波和传统溶热制备 UiO-66 材料用于高效储氢进行了比较研究。通过调节结晶温度和结晶时间，制备了不同结构和形态的 UiO-66。对微波法制备 UiO-66 的工艺进行了优化，获得了 120 ℃、1.0 h 的最佳制备条件，其比表面积为 1561 m2/g。为了深入了解该材料的储氢性能，我们建立了 UiO-66 的微观结构与其储氢性能之间的有效关联。实验结果表明，在 77 K 和 5 MPa 条件下，制备的 UiO-66 的吸氢率达到 3.78%。此外，还利用准一级、准二级动力学方程和颗粒内扩散模型定量描述了 UiO-66 吸氢过程的动力学规律和机理。本论文对UiO-66材料储氢的相关研究为MOFs材料的高效制备和储氢机理提供了理论依据和技术支持，为多孔材料固态储氢的应用提供了参考。

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Preparation and hydrogen storage properties of metal-organic framework UiO-66: Comparison of microwave and conventional hydrothermal preparation

The efficient preparation of metal-organic frameworks (MOFs) has become an important issue in the field of solid-state hydrogen storage due to the advantages of strong structural design and tunable pores of MOFs. However, its efficient preparation is still facing key bottlenecks such as process complexity, long cycle time and low efficiency. Microwave-assisted synthesis is an emerging technology that utilizes microwave external fields to enhance the mass and heat transfer and reaction behavior during the preparation of porous materials, thus promising to improve the preparation efficiency of MOFs materials. This method is considered to be an important development to realize the efficient preparation of MOFs materials. This work focuses on the comparative study of microwave and conventional solvothermal preparation of UiO-66 materials for efficient hydrogen storage. UiO-66 with different structures and morphologies were prepared by adjusting the crystallization temperature and crystallization time. The preparation process of UiO-66 by microwave method was optimized to obtain the optimal preparation conditions of 120 °C, 1.0 h, and its specific surface area of 1561 m²/g. In order to gain a deeper understanding of the hydrogen storage properties of the material, we have established an effective correlation between the microstructure of UiO-66 and its hydrogen storage properties. The experimental results showed that the hydrogen adsorption of the prepared UiO-66 reached 3.78% at 77 K and 5 MPa. In addition, quasi-primary and quasi-secondary kinetic equations and intra-particle diffusion models were used to quantitatively describe the kinetic laws and mechanisms of the hydrogen adsorption process of UiO-66. The research related to hydrogen storage in UiO-66 materials in this thesis provides theoretical basis and technical support for the efficient preparation and hydrogen storage mechanism of MOFs materials, and provides a reference for the application of solid-state hydrogen storage in porous materials.

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来源期刊

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.