以多金属氧酸盐为基础的共价有机骨架的构建和成型，以促进一罐CO2的转化

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2025-06-05 DOI:10.1002/aic.18927

Yi Yu, Xuquan Liu, Mingjian Shao, Jing Xiao, Chongxiong Duan, Hongxia Xi

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引用次数: 0

摘要

共价有机框架（COFs）作为一种潜在的多相催化剂，在一罐催化中面临着功能活性位点单一的问题。在此，一种多金属氧酸（POM）物质，磷酸钼酸水合物（PMA, H3PMo12O40）被稳定地整合到离子COF （EB‐TFP）的纳米笼中。考虑到实际应用，所得到的复合材料（EB‐TFP/PMA）粉末被塑造成具有足够的破碎强度和热稳定性的整体颗粒。这些材料用于二氧化碳和烯烃的一锅反应，得到了高附加值的环状碳酸盐。详细的活性评价表明，EB - TFP/PMA优异的催化性能（在80℃、1 bar、24 h和无共催化剂条件下，90%的主要产率）源于酸/碱位点的协同作用。该球团具有良好的催化性能（相同条件下产率为83%）和良好的可重复使用性。这项研究强调了COFs作为平台构建适合一锅催化的协同活性位点的潜力。

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Construction and shaping of polyoxometalate‐based covalent organic framework for boosting one‐pot CO2 conversion

Covalent organic frameworks (COFs), as potential heterogeneous catalysts, face the problem of single functional active sites in one‐pot catalysis. Herein, a polyoxometalate (POM) species, phosphomolybdic acid hydrate (PMA, H3PMo12O40) was stably integrated into the nanocages of an ionic COF (EB‐TFP). Considering practical applications, the resulting composite (EB‐TFP/PMA) powder was shaped into monolithic pellets with sufficient crushing strength and thermal stability. These materials were used in a one‐pot reaction of CO2 and olefins to obtain value‐added cyclic carbonates. Detailed activity evaluations revealed that the excellent catalytic performance (90% of main yield under the conditions of 80 C, 1 bar, 24 h and no co‐catalysts) of EB‐TFP/PMA arose from the synergistic effect of acid/base sites. The pellets also showed satisfactory catalytic performance (83% of yield under the same conditions) and good reusability. This study highlights the potential of COFs as platforms to construct synergistic active sites tailored for one‐pot catalysis.

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.