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Direct Identification of Mixed-Metal Centers in Metal-Organic Frameworks: Cu3(BTC)2 Transmetalated with Rh2+ Ions.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-09-07 , DOI: 10.1021/acs.jpclett.0c02539 Kamolrat Metavarayuth 1 , Otega Ejegbavwo 1 , Gavin McCarver 2 , Michael L Myrick 1 , Thomas M Makris 1 , Konstantinos D Vogiatzis 2 , Sanjaya D Senanayake 3 , Olivia M Manley 1 , Amani M Ebrahim 4 , Anatoly I Frenkel 3, 4 , Sooyeon Hwang 5 , Thayalan Rajeshkumar 2 , Juan D Jimenez 6 , Kexun Chen 1 , Natalia B Shustova 1 , Donna A Chen 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-09-07 , DOI: 10.1021/acs.jpclett.0c02539 Kamolrat Metavarayuth 1 , Otega Ejegbavwo 1 , Gavin McCarver 2 , Michael L Myrick 1 , Thomas M Makris 1 , Konstantinos D Vogiatzis 2 , Sanjaya D Senanayake 3 , Olivia M Manley 1 , Amani M Ebrahim 4 , Anatoly I Frenkel 3, 4 , Sooyeon Hwang 5 , Thayalan Rajeshkumar 2 , Juan D Jimenez 6 , Kexun Chen 1 , Natalia B Shustova 1 , Donna A Chen 1
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Raman spectroscopy was used to establish direct evidence of heterometallic metal centers in a metal–organic framework (MOF). The Cu3(BTC)2 MOF HKUST-1 (BTC3– = benzenetricarboxylate) was transmetalated by heating it in a solution of RhCl3 to substitute Rh2+ ions for Cu2+ ions in the dinuclear paddlewheel nodes of the framework. In addition to the Cu–Cu and Rh–Rh stretching modes, Raman spectra of (CuxRh1–x)3(BTC)2 show the Cu–Rh stretching mode, indicating that mixed-metal Cu–Rh nodes are formed after transmetalation. Density functional theory studies confirmed the assignment of a Raman peak at 285 cm–1 to the Cu–Rh stretching vibration. Electron paramagnetic resonance spectroscopy experiments further supported the conclusion that Rh2+ ions are substituted into the paddlewheel nodes of Cu3(BTC)2 to form an isostructural heterometallic MOF, and electron microscopy studies showed that Rh and Cu are homogeneously distributed in (CuxRh1–x)3(BTC)2 on the nanoscale.
中文翻译：
在金属-有机框架中直接识别混合金属中心：用Rh2 +离子金属化的Cu3（BTC）2。
拉曼光谱法用于建立金属-有机框架（MOF）中杂金属中心的直接证据。通过在RhCl 3溶液中加热Cu 3（BTC）2 MOF HKUST-1（BTC 3– =苯三羧酸酯）进行金属转移，以用Rh 2+离子代替框架的双核桨轮节点中的Cu 2+离子。除Cu–Cu和Rh–Rh拉伸模式外，（Cu x Rh 1– x）3（BTC）2的拉曼光谱示出了Cu–Rh的拉伸模式，表明在过渡金属化之后形成了混合金属Cu–Rh节点。密度泛函理论研究证实了Cu-Rh拉伸振动在285 cm -1处有一个拉曼峰。电子顺磁共振光谱实验进一步支持了将Rh 2+离子代入Cu 3（BTC）2的桨轮节点以形成同构异金属MOF的结论，并且电子显微镜研究表明Rh和Cu均匀分布在（Cu x Rh 1– x）3（BTC）2在纳米尺度上。
更新日期：2020-10-02
中文翻译：
在金属-有机框架中直接识别混合金属中心：用Rh2 +离子金属化的Cu3（BTC）2。
拉曼光谱法用于建立金属-有机框架（MOF）中杂金属中心的直接证据。通过在RhCl 3溶液中加热Cu 3（BTC）2 MOF HKUST-1（BTC 3– =苯三羧酸酯）进行金属转移，以用Rh 2+离子代替框架的双核桨轮节点中的Cu 2+离子。除Cu–Cu和Rh–Rh拉伸模式外，（Cu x Rh 1– x）3（BTC）2的拉曼光谱示出了Cu–Rh的拉伸模式，表明在过渡金属化之后形成了混合金属Cu–Rh节点。密度泛函理论研究证实了Cu-Rh拉伸振动在285 cm -1处有一个拉曼峰。电子顺磁共振光谱实验进一步支持了将Rh 2+离子代入Cu 3（BTC）2的桨轮节点以形成同构异金属MOF的结论，并且电子显微镜研究表明Rh和Cu均匀分布在（Cu x Rh 1– x）3（BTC）2在纳米尺度上。
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