Self‐Assembly Properties of NCN Pincer Palladium(II) Complexes Bearing a Uracil Moiety

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<jats:title>Abstract</jats:title><jats:p>NCN pincer palladium(II) complexes bearing a 6‐ethynyl‐1‐octyluracil moiety were designed by the combination of an NCN pincer palladium(II) complexes as an organometallic compound and a uracil derivative as a nucleobase to afford bioorganometallic compounds. The reaction of the NCN pincer ligand with Pd(dba)<jats:sub>2</jats:sub> (dba = dibenzylideneacetone) led to the formation of the NCN pincer palladium(II) complex <jats:bold>Pd‐Br</jats:bold>. The crystal structure of the cationic complex <jats:bold>Pd‐MeCN</jats:bold>, which was prepared by the treatment of <jats:bold>Pd‐Br</jats:bold> with AgOTf (OTf = trifluoromethanesulfonate) in acetonitrile, revealed that a dimeric structure formed through intermolecular hydrogen bonds between the uracil moieties of two independent molecules. The self‐assembly properties of the NCN pincer palladium(II) complexes were found to depend on the ancillary ligands. Each hydrogen‐bonded dimer was connected through an intermolecular hydrogen‐bonding bridge between the coordinated water molecule and the triflate anion in the cationic complex <jats:bold>Pd‐H<jats:sub>2</jats:sub>O</jats:bold>. Intermolecular hydrogen bonding between the uracil moiety and the triflate anion bound to the palladium center was observed in the NCN pincer palladium(II) complex <jats:bold>Pd‐OTf</jats:bold>, although a dimeric structure between the uracil moieties was formed in the NCN pincer palladium(II) complex <jats:bold>Pd‐O<jats:sub>2</jats:sub>CCF<jats:sub>3</jats:sub></jats:bold>, which was obtained by the abstraction of the bromide ion from <jats:bold>Pd‐Br</jats:bold> with AgO<jats:sub>2</jats:sub>CCF<jats:sub>3</jats:sub>.</jats:p>

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