Synthesis of Mixed-Metal MIL-68 under Mild Conditions by Controlling Nucleation Using a Microfluidic System
Synthesis of Mixed-Metal MIL-68 under Mild Conditions by Controlling Nucleation Using a Microfluidic System
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DOI：
10.1021/acs.cgd.2c00140
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发表时间：
2022-06
期刊：
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通讯作者：
Saki Yamada;A. Hirano;Yoko Tanaka;Ryohei Akiyoshi;Hirofumi Yoshikawa;D. Tanaka
中科院分区：
文献类型：
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作者：
Saki Yamada;A. Hirano;Yoko Tanaka;Ryohei Akiyoshi;Hirofumi Yoshikawa;D. Tanaka
以三价金属离子为结点的金属有机骨架(M3+-MOF)因其优异的热稳定性和化学稳定性而显示出广泛的应用潜力；然而，M3+-MOF的合成需要极端的反应条件，如高温、长时间的反应和添加氟化氢(HF)。在这里，我们通过微流控成核和金属混合的方法快速合成了含有三价金属离子的MIL-68分子筛。在Fe3+与配体的初始反应过程中，Al3+加成生成了一维链状二级结构单元，从而形成了MIL-68。与本体合成和微波辅助合成的产物相比，微流控合成的产物具有较高的结晶度。因此，将微流控系统与金属混合相结合是合成工业应用M3+-MOF的一种新方法。
Metal–organic frameworks that contain trivalent metal ions as nodes (M3+–MOFs) exhibit potential for various applications due to their exceptional thermal and chemical stability; however, M3+–MOF synthesis requires extreme reaction conditions such as high temperatures, long reaction times, and hydrogen fluoride (HF) addition. Here, we rapidly synthesized MIL-68 containing trivalent metal ions without any HF addition by controlling nucleation using microfluidic synthesis and metal mixing. Al3+addition during the initial reaction between Fe3+and the ligand yielded 1D chain-based secondary building units, consequently forming MIL-68. Compared to the products obtained using bulk and microwave-assisted syntheses, the product obtained via microfluidic synthesis exhibited high crystallinity. Thus, the combination of microfluidic systems and metal mixing is a novel approach in synthesizing industrially applicable M3+–MOFs.