Powering a CO2 Reduction Catalyst with Visible Light through Multiple Sub-picosecond Electron Transfers from a Quantum Dot
| Autor: | Shichen Lian, Dmitriy S. Dolzhnikov, Raul Calzada, Emily A. Weiss, Mohamad S. Kodaimati |
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| Rok vydání: | 2017 |
| Předmět: |
chemistry.chemical_element
02 engineering and technology General Chemistry 010402 general chemistry 021001 nanoscience & nanotechnology Photochemistry 01 natural sciences Biochemistry Redox Catalysis 0104 chemical sciences Electron transfer Colloid and Surface Chemistry chemistry Quantum dot Picosecond Iridium 0210 nano-technology Spectroscopy Visible spectrum |
| Zdroj: | Journal of the American Chemical Society. 139:8931-8938 |
| ISSN: | 1520-5126 0002-7863 |
| Popis: | Photosensitization of molecular catalysts to reduce CO2 to CO is a sustainable route to storable solar fuels. Crucial to the sensitization process is highly efficient transfer of redox equivalents from sensitizer to catalyst; in systems with molecular sensitizers, this transfer is often slow because it is gated by diffusion-limited collisions between sensitizer and catalyst. This article describes the photosensitization of a meso-tetraphenylporphyrin iron(III) chloride (FeTPP) catalyst by colloidal, heavy metal-free CuInS2/ZnS quantum dots (QDs) to reduce CO2 to CO using 450 nm light. The sensitization efficiency (turnover number per absorbed unit of photon energy) of the QD system is a factor of 18 greater than that of an analogous system with a fac-tris(2-phenylpyridine)iridium sensitizer. This high efficiency originates in ultrafast electron transfer between the QD and FeTPP, enabled by formation of QD/FeTPP complexes. Optical spectroscopy reveals that the electron-transfer processes primarily responsi... |
| Databáze: | OpenAIRE |
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