期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 47, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202211115
关键词
Electromerism; Low-Valent Silicon; Main Group; Silylene; Stimuli Responsive
资金
- state of Baden-Wurttemberg through bwHPC
- Deutsche Forschungsgemeinschaft (DFG) [INST 40/467-1 FUGG]
This study reports a stimuli-responsive low-valent silicon compound exhibiting a new phenomenon of electromerism in silicon chemistry, and the reaction is fully reversible.
Electromerism is a very well-known phenomenon in transition metal chemistry. In main group chemistry, this concept has only started getting attention recently. We report stimuli responsive low-valent silicon compounds exhibiting electromerism. A mixed-valent silaiminyl-silylene 1, [LSi-Si(NDipp)L] (L=PhC((NBu)-Bu-t)(2)), was synthesized in a single step from amidinate-chlorosilylene. Compound 1 has two interconnected Si atoms in formally +I and +III oxidation states. Upon treatment with Lewis acidic (CuX)-X-I (X=mesityl, Cl, Br, I), electron redistribution occurs resulting in the formation of [{LSi(NDipp)Si(L)}-CuX], in which both silicon atoms are in the +II formal oxidation state. Removal of the copper center from [{LSi(NDipp)Si(L)}-CuX] by using a Lewis basic carbene led to reformation of the precursor [LSi-Si(NDipp)L]. Thus, the process is fully reversible. This showcases the first example of Lewis acid/base-induced reversible electromerism in silicon chemistry.
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