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Models for reactions of acetylene on platinum(111): a vinyl(acetylene)triplatinum complex and evidence for an ethylidyne intermediate

Journal Article · · Organometallics; (United States)
DOI:https://doi.org/10.1021/om00097a029· OSTI ID:6969945

Reaction of (Pt/sub 3/(..mu../sub 3/-H)(..mu..-dppm)/sub 3/)/sup +/ (1) with excess acetylene gives (Pt/sub 3/(CH=CH/sub 2/)(..mu../sub 3/-eta/sup 2/(parallel)-HCCH)(..mu..-dppm)/sub 3/)/sup +/, where dppm = Ph/sub 2/PCH/sub 2/PPh/sub 2/. Deuterium-labeling studies indicate that H-D scrambling occurs within the vinyl group but not in the acetylene ligand. For example, (Pt/sub 3/(..mu../sub 3/-D)(..mu..-dppm)/sub 3/)/sup +/ with HCCH gave (Pt/sub 3/(CH==CH/sub 7/-d/sub 1/)(..mu../sub 3/-eta/sup 2/(parallel)-HCCH)(..mu..-dppm)/sub 3/)/sup +/, in which the deuterium label was distributed randomly in all three possible positions in the vinyl group. It is possible that this scrambling occurs by way of a short-lived ethylidyne intermediate. The complex is fluxional, due to rotation of the acetylene ligand, at room temperature. Similar reaction of 1 with excess propyne gives (Pt/sub 3/(CH=CHMe)(..mu../sub 3/-eta/sup 2/(**)-MeCCH)(..mu..-dppm)/sub 3/)/sup +/, but this complex is not fluxional at room temperature and is formed selectively by cis insertion of propyne into the Pt-H groups. There is a strong resemblance to the chemistry resulting from chemisorption of acetylene on a Pt(111) surface, thus providing a clear example of the value of coordinatively unsaturated clusters as mimics of metal surfaces.

Research Organization:
Univ. of Western Ontario, London (Canada)
OSTI ID:
6969945
Journal Information:
Organometallics; (United States), Journal Name: Organometallics; (United States) Vol. 7:7; ISSN ORGND
Country of Publication:
United States
Language:
English