Ambient Nucleation and Growth of Highly Crystalline Imine-Connected Covalent Organic Frameworks for Scalable Synthesis

IF 8.7 1区化学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Materials Letters Pub Date : 2025-07-17 DOI:10.1021/acsmaterialslett.5c00707

Xiaogeng Lin, Xingyu Ma, Shijun Li, Kaiyu Xiong and Lei Li*,

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Abstract

The exploration of facile polymerization strategies is critical for circumventing frustrating issues in the preparation of conventional covalent organic frameworks (COFs) and promoting their promising applications. Here, we report an ambient nucleation and growth strategy for synthesizing highly crystalline imine-connected COFs. The tetrahydrofuran/toluene cosolvent ensures the optimal dissolution of both monomers and oligomers, while aliphatic amine further enhances the solubility of aldehyde monomers and modulates the molecular assembly dynamically. Ordered COF nanosheets are observed in the early stage of polymerization, indicating the different nucleation mechanism from the predominant error-correction concept. This strategy demonstrates great versatility and robustness for 12 COFs with various functional groups and programmable topologies are successfully prepared, and near-theoretical surface areas in COF-TBDM and COF-TATA are achieved even in the large-scale (5 g) production batch. The effective integration of palladium nanoparticles (Pd NPs) on COF-TBDM is realized, resulting in a Pd@COF-TBDM catalyst with exceptional catalytic performance and stability during the nitro-hydrogenation reaction.

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可扩展合成高结晶亚胺连接共价有机骨架的环境成核和生长

探索易聚合策略对于避免传统共价有机框架（COFs）制备中令人沮丧的问题并促进其有前景的应用至关重要。在这里，我们报告了一种合成高结晶亚胺连接COFs的环境成核和生长策略。四氢呋喃/甲苯共溶剂保证了单体和低聚物的最佳溶解，而脂肪胺进一步提高了醛类单体的溶解度，并动态调节了分子组装。在聚合的早期阶段观察到有序的COF纳米片，表明与主流的误差校正概念不同的成核机制。该策略成功制备了12种具有不同官能团和可编程拓扑结构的cof，并且即使在大规模（5 g）生产批量中，COF-TBDM和COF-TATA的接近理论表面积也得到了实现。实现了钯纳米粒子（Pd NPs）在COF-TBDM上的有效整合，使得Pd@COF-TBDM催化剂在硝基加氢反应中具有优异的催化性能和稳定性。

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来源期刊

ACS Materials Letters MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

14.60

自引率

3.50%

发文量

261

期刊介绍： ACS Materials Letters is a journal that publishes high-quality and urgent papers at the forefront of fundamental and applied research in the field of materials science. It aims to bridge the gap between materials and other disciplines such as chemistry, engineering, and biology. The journal encourages multidisciplinary and innovative research that addresses global challenges. Papers submitted to ACS Materials Letters should clearly demonstrate the need for rapid disclosure of key results. The journal is interested in various areas including the design, synthesis, characterization, and evaluation of emerging materials, understanding the relationships between structure, property, and performance, as well as developing materials for applications in energy, environment, biomedical, electronics, and catalysis. The journal has a 2-year impact factor of 11.4 and is dedicated to publishing transformative materials research with fast processing times. The editors and staff of ACS Materials Letters actively participate in major scientific conferences and engage closely with readers and authors. The journal also maintains an active presence on social media to provide authors with greater visibility.