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Dehydrogenative polymerization of silanes to polysilanes by zirconocene and hafnocene catalysts. A new polymerization mechanism

Journal Article · · Journal of the American Chemical Society; (USA)
DOI:https://doi.org/10.1021/ja00202a070· OSTI ID:6725502
;  [1]
  1. Univ. of California, San Diego (USA)

Polysilanes, (-SiRR{prime}-){sub n} represent a class of inorganic polymers that have unusual chemical properties and a number of potential applications. Prospects for development of a coordination polymerization route to these polymers have improved dramatically with the recent discovery by Harrod and co-workers that titanocene and zirconocene alkyl derivatives are active catalysts for the dehydrogenative coupling of primary silanes RSiH{sub 3} to linear polysilanes with ca. 10-20 Si atoms (eq 1, Cp = {eta}{sup 5}-C{sub 5}H{sub 5}, M = Ti, Zr){sup 2}. We have found that a number of zirconium and hafnium silyl complexes of the type Cp{prime}{sub 2}M(SiR{sub 3})R{prime} (Cp{prime} = Cp, Cp* ({eta}{sup 5}-C{sub 5}Me{sub 5}); M = Zr, Hf; R = Me, Ph, SiMe{sub 3}; R{prime} = Cl, alkyl, silyl) are catalyst precursors for this dehydrogenative coupling reaction and that polymer molecular weights can vary as a function of reaction conditions and catalyst. This report describes observations that suggest a mechanism for dehydrogenative silane polymerization by zirconocene and hafnocene catalysts.

OSTI ID:
6725502
Journal Information:
Journal of the American Chemical Society; (USA), Journal Name: Journal of the American Chemical Society; (USA) Vol. 111:20; ISSN 0002-7863; ISSN JACSA
Country of Publication:
United States
Language:
English