Tuning the Catalytic Water Oxidation Activity through Structural Modifications of High-Nuclearity Mn-oxo Clusters [Mn18M] (M = Sr2+, Mn2+)
نویسندگان
چکیده
The water oxidation half-reaction is considered the bottleneck in development of technological advances to replace fossil fuels with sustainable and economically affordable energy sources. In natural photosynthesis, occurs oxygen evolving complex (OEC), a manganese-oxo cluster {Mn4CaO5} cubane-like topology that embedded within redox-active protein environment located photosystem II (PS II). Therefore, preparation biomimetic manganese-based compounds appealing for efficient inexpensive catalysts. Here, we present catalytic activity high-nuclearity mixed-metal manganese-strontium cluster, [MnIII12MnII6Sr(μ4-O8)(μ3-Cl)8(HLMe)12(MeCN)6]Cl2∙15MeOH (Mn18Sr) (HLMe = 2,6-bis(hydroxymethyl)-p-cresol), neutral media. This mixed-valence features different motifs it stabilized by redox-active, quinone-like organic ligands. displays low onset overpotential 192 mV overpotentials 284 550 at current densities 1 mA cm−2 10 cm−2, respectively. Direct O2 evolution measurements under visible light-driven conditions demonstrate capabilities this which exhibits turnover frequency 0.48 s−1 number 21.6. result allows direct comparison be made structurally analogous Mn-oxo [MnIII12MnII7(µ4-O)8(µ3-OCH3)2(µ3-Br)6(HLMe)12(MeOH)5(MeCN)]Br2·9MeCN·MeOH (Mn19), was recently reported us. work highlights potential series towards reaction their amenability induce structural changes modify reactivity.
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ژورنال
عنوان ژورنال: Water
سال: 2021
ISSN: ['2073-4441']
DOI: https://doi.org/10.3390/w13152042