NDLI: The Controlled Formation and Cleavage of an Intramolecular $d^{8}–d^{8}$ Pt–Pt Interaction in a Dinuclear Cycloplatinated Molecular “Pivot-Hinge”

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The Controlled Formation and Cleavage of an Intramolecular $d^{8}–d^{8}$ Pt–Pt Interaction in a Dinuclear Cycloplatinated Molecular “Pivot-Hinge”

Content Provider	World Health Organization (WHO)-Global Index Medicus
Author	Lau, Kai-cheung Koo, Chi-kin Wong, Wai-yeung Lam, Michael Hon-wah Wong, Ka-leung
Description	Author Affiliation: Koo CK ( Department of Chemistry and Biology, City University of Hong Kong, 83 Tat Chee Avenue, Hong Kong SAR, China.)
Abstract	The bis(diphenylphosphino)methane (dppm)-bridged dinuclear cycloplatinated complex $\{[Pt(L)]_{2}(μ-dppm)\}^{2+}$ $(Pt_{2}⋅dppm;$ HL: 2-phenyl-6-(1H-pyrazol-3-yl)-pyridine) demonstrates interesting reversible “pivot-hinge”-like intramolecular motions in response to the protonation/deprotonation of L. In its protonated “closed” configuration, the two platinum(II) centers are held in position by intramolecular $d^{8}–d^{8}$ Pt–Pt interaction. In its deprotonated “open” configuration, such Pt–Pt interaction is cleaved. To further understand the mechanism behind this hingelike motion, an analogous dinuclear cycloplatinated complex, $\{[Pt(L)]_{2}(μ-dchpm)\}^{2+}$ $(Pt_{2}⋅dchpm)$ with bis(dicyclohexylphosphino)methane (dchpm) as the bridging ligand, was synthesized. From its protonation/deprotonation responses, it was revealed that aromatic π–π interactions between the phenyl moieties of the μ-dppm and the deprotonated pyrazolyl rings of L was essential to the reversible cleavage of the intramolecular Pt–Pt interaction in $Pt_{2}⋅dppm.$ In the case of $Pt_{2}⋅dchpm,$ spectroscopic and spectrofluorometric titrations as well as X-ray crystallography indicated that the distance between the two platinum(II) centers shrank upon deprotonation, thus causing a redshift in its room-temperature triplet metal–metal-to-ligand charge-transfer emission from 614 to 625 nm. Ab initio calculations revealed the presence of intramolecular hydrogen bonding between the deprotonated and negatively charged 1-pyrazolyl-N moiety and the methylene CH and phenyl C–H of the μ-dppm. The “open” configuration of the deprotonated $Pt_{2}⋅dppm$ was estimated to be $19 kcal mol^{−1}$ more stable than its alternative “closed” configuration. On the other hand, the open configuration of the deprotonated $Pt_{2}⋅dchpm$ was $6 kcal mol^{−1}$ less stable than its alternative closed configuration.
ISSN	09476539
e-ISSN	15213765
Journal	Chemistry - A European Journal
Issue Number	31
Volume Number	15
Language	English
Publisher	Wiley-VCH;ChemPubSoc Europe
Publisher Date	2009-08-03
Publisher Place	Germany
Access Restriction	Open
Subject Keyword	Chemistry
Content Type	Text
Resource Type	Article
Subject	Organic Chemistry Catalysis

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