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• W4280528037 endingPage "8670" @default.
• W4280528037 startingPage "8657" @default.
• W4280528037 abstract "In the present study, a series of non-chelated BTD (2,1,3-benzothiadiazole)-bridged diruthenium(II) ([{(CH3CN)(acac)2RuII}2(μ-BTD)] 1, [{CH3CN(acac)2RuII}(μ-BTD){RuII(acac)2(η1-N-BTD)}] 2, [{(η1-N-BTD)(acac)2RuII}2(μ-BTD)] 3), and triruthenium ([{(acac)2RuII}3(μ-BTD)2(η1-N-BTD)2] 4) complexes with varying ratios of η1-N and μ-bis-η1-N,η1-N modes of BTD were studied. Complexes 1-4 (S = 0) were obtained via the one-pot reaction of electron-rich Ru(acac)2(CH3CN)2 and electron-deficient BTD in refluxing acetone. The relatively low Ru(II)/Ru(III) potential of 1-4 (0.08-0.44 V versus SCE) further facilitated the isolation of the corresponding mixed valent RuIIRuIII (S = 1/2) and RuIIRuIIRuIII (S = 1/2)/RuIIRuIIIRuIII (S = 1) forms [1]ClO4-[3]ClO4 and [4]ClO4/[4](ClO4)2, respectively. The single-crystal X-ray structures of the representative mixed valent [1]ClO4 and [3]ClO4 established (i) Ru⋯Ru distances of 6.227 Å and 6.256 Å (molecule A)/6.184 Å (molecule B), respectively, (ii) a significant variation of the N-S distance of BTD in [3]ClO4 as a function of its binding mode μ versus η1 and (iii) similar Ru-N (μ-BTD) distances in each case corresponding to a valence delocalised situation. The mixed valent diruthenium (1+-3+) and triruthenium (4+/42+) complexes exhibited metal-based anisotropic electron paramagnetic resonance (EPR) and moderately intense low-energy intervalence charge-transfer (IVCT) transitions in the near-infrared region of 1730-1890 nm. Analysis of the IVCT band using the Hush treatment revealed a valence delocalised class III mixed valent state with the electronic coupling Vab of ≈2640-2890 cm-1, as also corroborated by the Kc values of 105-108, solvent independency of the IVCT band and uniform spin distribution between the metal ions in the singly occupied state(s). Furthermore, the involvement of the BTD (η1 and μ)-based orbitals in the reduction processes was evident by its free radical EPR feature." @default.
• W4280528037 created "2022-05-22" @default.
• W4280528037 creator A5011656913 @default.
• W4280528037 creator A5014287826 @default.
• W4280528037 creator A5062826786 @default.
• W4280528037 creator A5082807868 @default.
• W4280528037 date "2022-01-01" @default.
• W4280528037 modified "2023-10-16" @default.
• W4280528037 title "Diruthenium and triruthenium compounds of the potential redox active non-chelated η¹-N,η¹-N-benzothiadiazole bridge" @default.
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• W4280528037 doi "https://doi.org/10.1039/d2dt00533f" @default.
• W4280528037 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/35583102" @default.
• W4280528037 hasPublicationYear "2022" @default.

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