Tetrazine Chelate Ligands Bridging Two [Ru(acac)2] Fragments: Mixed Valency and Radical Complex Formation
Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1, 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the complexes 3=[Ru(acac)2(1)], 4={[Ru(acac)2]2(1)], 5={[Ru(acac)2]2(bmtz)], and 6={[Ru(acac)2]2(2)] were prepared and identified by structure analy...
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| Vydané v: | Zeitschrift für anorganische und allgemeine Chemie (1950) Ročník 648; číslo 23 |
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| Hlavní autori: | , , , , , |
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| Jazyk: | English |
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| Abstract | Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1, 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the complexes 3=[Ru(acac)2(1)], 4={[Ru(acac)2]2(1)], 5={[Ru(acac)2]2(bmtz)], and 6={[Ru(acac)2]2(2)] were prepared and identified by structure analysis of crystallized material. The one‐electron oxidized form 6(PF6) was also studied structurally, suggesting a Class II mixed‐valent situation. The neutral dinuclear systems exhibit two reversible oxidation processes with comproportionation constants 109.2<Kc<1014.1 and one reduction which were analyzed UV/vis/NIR and EPR spectroscopically. Oxidation produces largely metal‐based mixed‐valent cations with very weak intervalence absorptions in the near IR whereas the electron uptake occurs at the tetrazine acceptor. |
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| AbstractList | Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1, 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the complexes 3=[Ru(acac)2(1)], 4={[Ru(acac)2]2(1)], 5={[Ru(acac)2]2(bmtz)], and 6={[Ru(acac)2]2(2)] were prepared and identified by structure analysis of crystallized material. The one‐electron oxidized form 6(PF6) was also studied structurally, suggesting a Class II mixed‐valent situation. The neutral dinuclear systems exhibit two reversible oxidation processes with comproportionation constants 109.2<Kc<1014.1 and one reduction which were analyzed UV/vis/NIR and EPR spectroscopically. Oxidation produces largely metal‐based mixed‐valent cations with very weak intervalence absorptions in the near IR whereas the electron uptake occurs at the tetrazine acceptor.Dedicated to Thomas Schleid, Schoolmate and Colleague, on the Occasion of his 65th Birthday Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1 , 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the complexes 3 =[Ru(acac) 2 ( 1 )], 4 ={[Ru(acac) 2 ] 2 ( 1 )], 5 ={[Ru(acac) 2 ] 2 (bmtz)], and 6 ={[Ru(acac) 2 ] 2 ( 2 )] were prepared and identified by structure analysis of crystallized material. The one‐electron oxidized form 6 (PF 6 ) was also studied structurally, suggesting a Class II mixed‐valent situation. The neutral dinuclear systems exhibit two reversible oxidation processes with comproportionation constants 10 9.2 < K c <10 14.1 and one reduction which were analyzed UV/vis/NIR and EPR spectroscopically. Oxidation produces largely metal‐based mixed‐valent cations with very weak intervalence absorptions in the near IR whereas the electron uptake occurs at the tetrazine acceptor. Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1, 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the complexes 3=[Ru(acac)2(1)], 4={[Ru(acac)2]2(1)], 5={[Ru(acac)2]2(bmtz)], and 6={[Ru(acac)2]2(2)] were prepared and identified by structure analysis of crystallized material. The one‐electron oxidized form 6(PF6) was also studied structurally, suggesting a Class II mixed‐valent situation. The neutral dinuclear systems exhibit two reversible oxidation processes with comproportionation constants 109.2<Kc<1014.1 and one reduction which were analyzed UV/vis/NIR and EPR spectroscopically. Oxidation produces largely metal‐based mixed‐valent cations with very weak intervalence absorptions in the near IR whereas the electron uptake occurs at the tetrazine acceptor. |
| Author | Filippou, Vasileios Schwederski, Brigitte Fiedler, Jan Ringenberg, Mark R. Kaim, Wolfgang Löw, Isabell |
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| Cites_doi | 10.1021/ic00111a045 10.1002/chem.201501726 10.1016/S0898-8838(08)60174-9 10.1021/ic00307a020 10.1039/D0DT00827C 10.1515/znb-1995-0123 10.1002/anie.200501075 10.1021/ic001228q 10.1002/anie.200602737 10.1039/b407611g 10.1021/ja077676f 10.1016/S0065-2792(08)60179-X 10.1039/P29930002109 10.1021/ic00280a010 10.1039/b500152h 10.1021/acs.inorgchem.7b01812 10.1039/b504286k 10.1002/9780470166314.ch1 10.1016/j.ccr.2006.06.003 10.1021/ic980576d 10.1021/ja982673b 10.1002/ange.200602737 10.1002/ange.200501075 |
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| Snippet | Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1, 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the... Using bis(3‐methyl‐2‐pyridyl)‐1,2,4,5‐tetrazine 1 , 3‐(2‐pyrimidyl)‐6‐methyl‐1,2,4,5‐tetrazine 2 and bis(2‐pyrimidyl)‐1,2,4,5‐tetrazine=bmtz as ligands, the... |
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| SubjectTerms | Complex formation Crystal structure Crystallization Cyclic voltammetry Diruthenium compounds EPR spectroscopy Ligands Oxidation Spectroelectrochemistry Structural analysis |
| Title | Tetrazine Chelate Ligands Bridging Two [Ru(acac)2] Fragments: Mixed Valency and Radical Complex Formation |
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