Ott Jonas C, Wadepohl Hubert, Enders Markus, Gade Lutz H
Anorganisch-Chemisches Institut , Universität Heidelberg , Im Neuenheimer Feld 276 , 69120 Heidelberg , Germany.
J Am Chem Soc. 2018 Dec 19;140(50):17413-17417. doi: 10.1021/jacs.8b11330. Epub 2018 Dec 5.
Guided by DFT based modeling the chemical shift range of a hydride resonance in the proton nuclear magnetic resonance (NMR) spectrum of the intermediate-spin, square planar iron complex (PNP)Fe-H was predicted and detected as a broad resonance at -3560 ppm (295 K) with a temperature dependent shift of approximately 2000 ppm between 223 and 383 K. The first detection of a metal-bonded hydrogen atom by solution NMR in a complex with a paramagnetic ground state illustrates the interplay of theory and experiment for the characterization of key components in paramagnetic base metal catalysis.
在基于密度泛函理论（DFT）的建模指导下，预测并检测到了中间自旋的平面正方形铁配合物(PNP)Fe-H的质子核磁共振（NMR）谱中氢化物共振的化学位移范围，其在-3560 ppm（295 K）处为宽共振峰，在223至383 K之间温度依赖性位移约为2000 ppm。通过溶液NMR首次在具有顺磁性基态的配合物中检测到金属键合的氢原子，这说明了理论与实验在顺磁性贱金属催化关键成分表征中的相互作用。
