Amphiphilic Polycarbonate Micellar Rhenium Catalysts for Efficient Photocatalytic CO2 Reduction in Aqueous Media

A triblock amphiphilic polymer derived from the copolymerization of CO2 and epoxides containing a bipyridine rhenium complex in its backbone is shown to effectively catalyze the visible‐light‐driven reduction of CO2 to CO. This polymer provides uniformly spherical micelles in aqueous solution, where...

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Published inAngewandte Chemie International Edition Vol. 61; no. 27; pp. e202200751 - n/a
Main Authors Ren, Fang‐Yu, Chen, Kaihong, Qiu, Li‐Qi, Chen, Jin‐Mei, Darensbourg, Donald J., He, Liang‐Nian
Format Journal Article
LanguageEnglish
Published Weinheim Wiley Subscription Services, Inc 04.07.2022
EditionInternational ed. in English
Subjects
Amphiphilic Micelles
Aqueous Media
Aqueous solutions
Carbon dioxide
Carbon monoxide
Catalysts
Chemical reduction
CO2 Reduction
Copolymerization
Deactivation
Epoxides
Hydrogen production
Hydrophobicity
Micelles
Organic chemistry
Photocatalysis
Polycarbonate
Polycarbonate resins
Polymers
Rhenium
Selectivity
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Summary:A triblock amphiphilic polymer derived from the copolymerization of CO2 and epoxides containing a bipyridine rhenium complex in its backbone is shown to effectively catalyze the visible‐light‐driven reduction of CO2 to CO. This polymer provides uniformly spherical micelles in aqueous solution, where the metal catalyst is sequestered in the hydrophobic portion of the nanostructured micelle. CO2 to CO reduction occurs in an efficient visible‐light‐driven process in aqueous media with turnover numbers up to 110 (>99 % selectivity) in the absence of a photosensitizer, which is a 37‐fold enhancement over the corresponding molecular rhenium catalyst in organic solvent. Notably, the amphiphilic polycarbonate micelle rhenium catalyst suppresses H2 generation, presumably by preventing deactivation of the active catalytic center by water. Visible‐light‐induced photocatalytic CO2 reduction in aqueous media was achieved with amphiphilic polycarbonate micellar rhenium catalysts. Coordination polymers were prepared comprising amphiphilic micelles with tunable solubility in water. By adjusting the proportion of hydrophilic and hydrophobic segments, the photocatalytic system was tailored to select for CO evolution.
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ISSN:1433-7851
1521-3773
DOI:10.1002/anie.202200751