Design of an inherently-stable water oxidation catalyst

Biswarup Chakraborty, Gal Gan-Or, Manoj Raula, Eyal Gadot, Ira A. Weinstock

פרסום מחקרי: פרסום בכתב עתמאמרביקורת עמיתים

תקציר

While molecular water-oxidation catalysts are remarkably rapid, oxidative and hydrolytic processes in water can convert their active transition metals to colloidal metal oxides or hydroxides that, while quite reactive, are insoluble or susceptible to precipitation. In response, we propose using oxidatively-inert ligands to harness the metal oxides themselves. This approach is demonstrated by covalently attaching entirely inorganic oxo-donor ligands (polyoxometalates) to 3-nm hematite cores, giving soluble anionic structures, highly resistant to aggregation, yet thermodynamically stable to oxidation and hydrolysis. Using orthoperiodate (at pH 8), and no added photosensitizers, the hematite-core complex catalyzes visible-light driven water oxidation for seven days (7600 turnovers) with no decrease in activity, far exceeding the documented lifetimes of molecular catalysts under turnover conditions in water. As such, a fundamental limitation of molecular complexes is entirely bypassed by using coordination chemistry to harness a transition-metal oxide as the reactive center of an inherently stable, homogeneous water-oxidation catalyst.

שפה מקוריתאנגלית אמריקאית
מספר המאמר4896
כתב עתNature Communications
כרך9
מספר גיליון1
מזהי עצם דיגיטלי (DOIs)
סטטוס פרסוםפורסם - 1 דצמ׳ 2018

ASJC Scopus subject areas

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  • ???subjectarea.asjc.1300.1300???
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