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Novel dirhodium coordination polymers: the impact of side chains on cyclopropanation†
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2018-09-05 00:00:00 , DOI: 10.1039/c8cy01493k Jiquan Liu 1, 2, 3, 4, 5 , Yeping Xu 6, 7, 8, 9 , Pedro B. Groszewicz 6, 7, 8, 9 , Martin Brodrecht 6, 7, 8, 9 , Claudia Fasel 7, 8, 9, 10 , Kathrin Hofmann 6, 7, 8, 9 , Xijuan Tan 5, 11, 12, 13, 14 , Torsten Gutmann 6, 7, 8, 9 , Gerd Buntkowsky 6, 7, 8, 9
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2018-09-05 00:00:00 , DOI: 10.1039/c8cy01493k Jiquan Liu 1, 2, 3, 4, 5 , Yeping Xu 6, 7, 8, 9 , Pedro B. Groszewicz 6, 7, 8, 9 , Martin Brodrecht 6, 7, 8, 9 , Claudia Fasel 7, 8, 9, 10 , Kathrin Hofmann 6, 7, 8, 9 , Xijuan Tan 5, 11, 12, 13, 14 , Torsten Gutmann 6, 7, 8, 9 , Gerd Buntkowsky 6, 7, 8, 9
Affiliation
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Seven novel dirhodium coordination polymers (Rh2–Ln) (n = 1–7) are prepared by employing bitopic ligands to connect dirhodium nodes. The formation of the framework is confirmed by attenuated total reflectance Fourier transform infrared (ATR-FTIR) and 1H → 13C cross polarization magic angle spinning nuclear magnetic resonance (CP MAS NMR) spectroscopy. Defect sites resulting from incomplete ligand substitution are revealed by 19F MAS NMR. The random stacking behavior of the frameworks in the obtained solid is analyzed by scanning electron microscopy (SEM) and X-ray diffraction (XRD). The Rh2/O interaction in neighboring layers is investigated by diffuse reflectance ultra-violet visible light (DR-UV-vis) spectroscopy and X-ray photoelectron spectroscopy (XPS). This interaction is relevant to understand the catalytic behavior of various Rh2–Ln catalysts in the cyclopropanation of styrene with ethyl diazoacetate (EDA). In this context, the structure-reactivity relationship is discussed by taking into consideration both interlayer Rh2/O interactions and steric effects of side chains.
中文翻译：
新型dirhodium配位聚合物：侧链对环丙烷化的影响†
通过使用双位配体连接dirhodium节点，制备了七个新颖的dirhodium配位聚合物（Rh 2 -L n）（n = 1-7）。通过衰减的全反射傅立叶变换红外光谱（ATR-FTIR）和1 H→ 13 C交叉极化魔角旋转核磁共振（CP MAS NMR）光谱确认了骨架的形成。19 F MAS NMR揭示了由于配体取代不完全而导致的缺陷位点。通过扫描电子显微镜（SEM）和X射线衍射（XRD）分析所获得的固体中骨架的无规堆积行为。Rh 2通过漫反射率紫外可见光（DR-UV-vis）光谱和X射线光电子能谱（XPS）研究邻近层中的/ O相互作用。这种相互作用对于了解各种Rh 2 -L n催化剂在苯乙烯与重氮乙酸乙酯（EDA）的环丙烷化中的催化性能有关。在这种情况下，通过考虑层间Rh 2 / O相互作用和侧链的空间效应来讨论结构-反应性关系。
更新日期：2018-09-05
中文翻译：
新型dirhodium配位聚合物：侧链对环丙烷化的影响†
通过使用双位配体连接dirhodium节点，制备了七个新颖的dirhodium配位聚合物（Rh 2 -L n）（n = 1-7）。通过衰减的全反射傅立叶变换红外光谱（ATR-FTIR）和1 H→ 13 C交叉极化魔角旋转核磁共振（CP MAS NMR）光谱确认了骨架的形成。19 F MAS NMR揭示了由于配体取代不完全而导致的缺陷位点。通过扫描电子显微镜（SEM）和X射线衍射（XRD）分析所获得的固体中骨架的无规堆积行为。Rh 2通过漫反射率紫外可见光（DR-UV-vis）光谱和X射线光电子能谱（XPS）研究邻近层中的/ O相互作用。这种相互作用对于了解各种Rh 2 -L n催化剂在苯乙烯与重氮乙酸乙酯（EDA）的环丙烷化中的催化性能有关。在这种情况下，通过考虑层间Rh 2 / O相互作用和侧链的空间效应来讨论结构-反应性关系。
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