Defect engineering: an effective tool for enhancing the catalytic performance of copper-MOFs for the click reaction and the A(3) coupling

Fan Zhiying; Wang Zheng; Cokoja MirzaFischer Roland A.

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Defect engineering: an effective tool for enhancing the catalytic performance of copper-MOFs for the click reaction and the A(3) coupling

机译：缺陷工程:一个有效的工具增强的催化性能点击反应和copper-MOFs (3)耦合

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A series of Cu(I)-enriched metal-organic frameworks (MOF) of the type CuBTC (BTC = benzene-1,3,5-tricarboxylate) was prepared by a mixed-linker defect engineering technique, namely substituting a portion of a parent linker with truncated pyridine-3,5-dicarboxylate (PyDC) in the synthesis process. The reduced carboxyl coordination sites and the emerged Lewis basic pyridyl sites of PyDC spawned mixed-valence Cu(I)-Cu(II) paddlewheels (PWs) in the defect-engineered CuBTC (DE-CuBTC) structure. Cu(I)-enriched DE-CuBTC shows significantly enhanced catalytic performance for the click reaction of azide-alkyne cycloaddition by accelerating the rate determining step of Cu(I)-acetylide intermediate formation. To further evaluate the catalytic activity of Cu(I)-enriched DE-CuBTC for reactions involving a Cu(I)-acetylide intermediate, the A(3) coupling reaction of phenylacetylene, paraformaldehyde and piperidine was studied as well. This study shows that defect engineering is an effective editing tool of catalytic active sites in catalysts.

机译：一系列的铜(I)纯度的浓缩铀的有机配合框架(MOF)的类型CuBTC (BTC =benzene-1 3 5-tricarboxylate)是由一个准备的mixed-linker缺陷工程技术,即代替父母链接器的一部分截断pyridine-3 5-dicarboxylate (PyDC)合成过程。协调网站和出现刘易斯的基本吡啶基PyDC催生了混合价的网站铜(I)铜(II)明轮(PWs)defect-engineered CuBTC (DE-CuBTC)结构。铜(I)纯度的浓缩铀DE-CuBTC显示显著单击增强的催化性能azide-alkyne环加成反应加速的速率决定步骤铜(I)乙炔化物中间体的形成。进一步评估的催化活性铜(I)纯度的浓缩铀DE-CuBTC反应涉及铜(I)乙炔化物中间体,(3)耦合苯乙炔反应、多聚甲醛和哌啶进行了研究。缺陷工程是一种有效的编辑催化剂的催化活性位点的工具。

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来源
《Catalysis science & technology》 |2021年第7期|2396-2402|共7页
作者
Fan Zhiying; Wang Zheng; Cokoja MirzaFischer Roland A.;
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作者单位

Northwest Univ, Coll Food Sci & Engn, Xian 710127, Peoples R China;

Tech Univ Munich, Chair Inorgan & Metal Organ Chem, Catalysis Res Ctr, Ernst Otto Fischer Str 1, D-85748 Garching, Germany;

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正文语种英语
中图分类汉语教学;
关键词
Catalysis; piperidine; EngineeringREACTIONclicking;

机译：催化;哌啶;EngineeringREACTIONclicking;

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Defect engineering: an effective tool for enhancing the catalytic performance of copper-MOFs for the click reaction and the A(3) coupling

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