FULL PAPER DOI:10.1002/ejic.201402954 Platinum Diolefin Complexes – Synthesis, Structures, and Cytotoxicity Anna Lüning, [a] Michael Neugebauer, [a] Verena Lingen, [a,b] Alexander Krest, [a] Kathrin Stirnat, [a] Glen B. Deacon, [b] Penny R. Drago, [b] Ingo Ott, [c] Julia Schur, [c] Ingo Pantenburg, [a] Gerd Meyer, [a] and Axel Klein* [a] Dedicated to Professor Hubert Schmidbaur on the occasion of his 80th birthday Keywords: Platinum / Alkene ligands / Structure elucidation / Structure–activity relationships / Cytotoxicity The synthesis, spectroscopy, structures and chemical reac- tivity of platinum(II) diolefin complexes cis-[(|| ||)PtCl 2 ], cis- [(|| ||)PtCl(R)] and cis-[(|| ||)Pt(R) 2 ] [|| || = chelate diolefin li- gand: 1,5-cyclooctadiene (COD), 1,5-dimethylocta-1,5-diene (Me 2 COD), norbornadiene (NBD), 1,5-hexadiene (HEX), 3- allyloxypropene (All 2 O, diallyl ether), diallylamine (All 2 NH); R = Me, Bn, C 6 F 5 ,C 6 F 4 H-4 (or -5), or CC(4-Me)Ph] have been explored. The relative exchange rates of the cis-[(|| ||)- PtCl 2 ] complexes towards the diimine ligand diisopropyl-1,4- diazabutadiene (iPr-DAB) increased along the series COD Me 2 COD NBD HEX All 2 O by a factor of 4. The pre- sumably dimeric complex [(All 2 NH)PtCl 2 ] 2 undergoes a unique rearrangement process in dimethyl sulfoxide (DMSO) Introduction The binding of olefins to transition metal ions reveals a marked maximum of stability for platinum(II) and palla- dium(II). This observation can be explained from the best match of promotion energy (should be low) and electron affinity (should be high). [1,2] Given the inert nature of Pt II , it is unsurprising that Zeise prepared K[PtCl 3 (C 2 H 4 )] (Zeise’s salt) in 1827, which is considered to be the first organometallic complex. [2–5] The Pd II derivative [PdCl 3 (C 2 H 4 )] plays a crucial role in one of the most im- portant industrial chemical processes, that is, the oxidation [a] Universität zu Köln, Department für Chemie, Institut für Anorganische Chemie, Greinstrasse 6, 50939 Köln, Germany E-mail: axel.klein@uni-koeln.de http://www.klein.uni-koeln.de/ [b] School of Chemistry, Monash University, P. O. Box 23, VIC 3800, Australia [c] Institute of Medicinal and Pharmaceutical Chemistry, Technische Universität Braunschweig, Beethovenstraße 55, 38106 Braunschweig, Germany Supporting information for this article is available on the WWW under http://dx.doi.org/10.1002/ejic.201402954. Eur. J. Inorg. Chem. 2015, 226–239 © 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim 226 solution to yield the dimeric piperazine complex [PtCl(dmso)- (C 6 H 10 N)] 2 , which has been characterised by single-crystal XRD. For selected platinum complexes, cytotoxic effects in HT-29 colon carcinoma and MCF-7 breast cancer cell lines were evaluated. For comparison, the dicationic complexes [(COD)Pt(Bn)(L)][PF 6 ] 2 with the very labile coligands N- methyl-4,4'-bipyridinium (MQ + ) and N-methyl-1,4-pyrazin- ium (Mpz + ) were added to the study. Although the hexadiene complexes [(HEX)Pt(C 6 F 4 H-4) 2 ] and [(HEX)Pt(C 6 F 4 H-5) 2 ] show strong cytotoxicity, the introduction of labile diolefin ligands or the labile cationic MQ + or Mpz + coligands does not generally lead to markedly increased cytotoxicity. of ethane in the so-called Wacker–Hoechst process (also Wacker oxidation). [6] To enhance the stability of olefin platinum complexes, the chelate effect is crucial, and 1,5-cyclooctadiene (COD) is best for this purpose. The relatively high stability of COD complexes opens several routes for the derivatisation of the frequently used starting complex [(COD)PtCl 2 ] (Scheme 1). Firstly, the quite stable CODPt scaffold allows the replace- ment of one or two Cl coligands by carbanionic coligands, such as alkyl, [7–13] aryl, [10–14] alkynyl, [13–18] alkenyl [16,19] or cyclopentadienide, [20] to form various derivatives (Scheme 1, Reaction 1) or by other anionic coligands such as amides, [21] thiolates, [22,23] SCN or pseudohalides (Scheme 1, Reaction 2). [7,10,22,24] The limit of this reaction is set by strong nucleophiles (Nu), which attack the olefin double bond to yield a Pt–C–C–Nu unit with a Pt–C σ bond. [7,25,26] Neutral coligands can be introduced by ab- straction of a Cl ion with Ag + or Tl + salts to yield cationic complexes (Scheme 1, Reaction 3). [13,14,26] The choice of an appropriate ligand even allows the introduction of a monoanionic chelate ligand for the two Cl coligands, [27] whereas reactions with neutral chelate ligands lead to the