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• W3166686855 endingPage "9620" @default.
• W3166686855 startingPage "9607" @default.
• W3166686855 abstract "This article deals with the development of the unprecedented redox-mediated heterometallic coordination polymer {[RuIII(acac)2(μ-bis-η1-N,η1-N-BTD)2AgI(ClO4)]ClO4}n (3) via the oxidation of the monomeric building block cis-[RuII(acac)2(η1-N-BTD)2] (1) by AgClO4 (BTD = exodentate 2,1,3-benzothiadiazole, acac = acetylacetonate). Monomeric cis-[RuII(acac)2(η1-N-BTD)2] (1) and [RuII(acac)2(η1-N-BTD)(CH3CN)] (2) were simultaneously obtained from the electron-deficient BTD heterocycle and the electron-rich metal precursor RuII(acac)2(CH3CN)2 in refluxing CH3CN. Molecular identities of 1–3 were authenticated by their single-crystal X-ray structures as well as by solution spectral features. These results also reflected the elusive trigonal-planar geometry of the Ag ion in Ru–Ag-derived polymeric 3. Ru(III) (S = 1/2)-derived 3 displayed metal-based anisotropic EPR with ⟨g⟩/Δg = 2.12/0.56 and paramagnetically shifted 1H NMR. Spectroelectrochemistry in combination with DFT/TD-DFT calculations of 1n and 2n (n = 1+, 0, 1–) determined a metal-based (RuII/RuIII) oxidation and BTD-based reduction (BTD/BTD•–). The drastic decrease in the emission intensity and quantum yield but insignificant change in the lifetime of 3 with respect to 1 could be addressed in terms of static quenching and/or a paramagnetism-induced phenomenon. A homogeneously dispersed dumbbell-shaped morphology and the particle diameter of 3 were established by microscopic (TEM-EDX/SEM) and DLS analysis, respectively. Moreover, the dynamic nature of polymeric 3 was highlighted by its degradation to the η1-N-BTD coordinated monomeric fragment 1, which could also be followed spectrophotometrically in polar protic EtOH. Interestingly, both monomeric 1 and polymeric 3 exhibited efficient electrocatalytic activity toward water oxidation processes (OER, HER) on immobilization on an FTO support, which also divulged the better intrinsic water oxidation activity of 3 in comparison to 1." @default.
• W3166686855 created "2021-06-22" @default.
• W3166686855 creator A5011656913 @default.
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• W3166686855 creator A5086841552 @default.
• W3166686855 date "2021-06-14" @default.
• W3166686855 modified "2023-10-03" @default.
• W3166686855 title "Ruthenium–Benzothiadiazole Building Block Derived Dynamic Heterometallic Ru–Ag Coordination Polymer and Its Enhanced Water-Splitting Feature" @default.
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• W3166686855 doi "https://doi.org/10.1021/acs.inorgchem.1c00865" @default.
• W3166686855 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/34121388" @default.

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