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Ultrafast Electron ...
Ultrafast Electron Transfer from CuInS2 Quantum Dots to a Molecular Catalyst for Hydrogen Production : Challenging Diffusion Limitations
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- Bagnall, Andrew J. (författare)
- Uppsala universitet,Fysikalisk kemi,Univ Grenoble Alpes, CNRS, Lab Chim & Biol Met, CEA,IRIG, F-38054 Grenoble, France.
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- Eliasson, Nora (författare)
- Uppsala universitet,Fysikalisk kemi
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- Hansson, Sofie (författare)
- Uppsala universitet,Institutionen för kemi - BMC
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- Chavarot-Kerlidou, Murielle (författare)
- Univ Grenoble Alpes, CNRS, Lab Chim & Biol Met, CEA,IRIG, F-38054 Grenoble, France.
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- Artero, Vincent (författare)
- Univ Grenoble Alpes, CNRS, Lab Chim & Biol Met, CEA,IRIG, F-38054 Grenoble, France.
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- Tian, Haining, 1983- (författare)
- Uppsala universitet,Fysikalisk kemi
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- Hammarström, Leif, 1964- (författare)
- Uppsala universitet,Fysikalisk kemi
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(creator_code:org_t)
- 2024
- 2024
- Engelska.
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Ingår i: ACS Catalysis. - 2155-5435. ; 14:6, s. 4186-4201
- Relaterad länk:
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https://doi.org/10.1...
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https://uu.diva-port... (primary) (Raw object)
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- Systems integrating quantum dots with molecular catalysts are attracting ever more attention, primarily owing to their tunability and notable photocatalytic activity in the context of the hydrogen evolution reaction (HER) and CO2 reduction reaction (CO2RR). CuInS2 (CIS) quantum dots (QDs) are effective photoreductants, having relatively high-energy conduction bands, but their electronic structure and defect states often lead to poor performance, prompting many researchers to employ them with a core–shell structure. Molecular cobalt HER catalysts, on the other hand, often suffer from poor stability. Here, we have combined CIS QDs, surface-passivated with l-cysteine and iodide from a water-based synthesis, with two tetraazamacrocyclic cobalt complexes to realize systems which demonstrate high turnover numbers for the HER (up to >8000 per catalyst), using ascorbate as the sacrificial electron donor at pH = 4.5. Photoluminescence intensity and lifetime quenching data indicated a large degree of binding of the catalysts to the QDs, even with only ca. 1 μM each of QDs and catalysts, linked to an entirely static quenching mechanism. The data was fitted with a Poissonian distribution of catalyst molecules over the QDs, from which the concentration of QDs could be evaluated. No important difference in either quenching or photocatalysis was observed between catalysts with and without the carboxylate as a potential anchoring group. Femtosecond transient absorption spectroscopy confirmed ultrafast interfacial electron transfer from the QDs and the formation of the singly reduced catalyst (CoII state) for both complexes, with an average electron transfer rate constant of ≈ (10 ps)−1. These favorable results confirm that the core tetraazamacrocyclic cobalt complex is remarkably stable under photocatalytic conditions and that CIS QDs without inorganic shell structures for passivation can act as effective photosensitizers, while their smaller size makes them suitable for application in the sensitization of, inter alia, mesoporous electrodes.
Ämnesord
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
Nyckelord
- hydrogen
- photocatalysis
- copper indium sulfide
- quantum dots
- molecular catalyst
- transient absorption
- artificial photosynthesis
- Chemistry with specialization in Physical Chemistry
- Kemi med inriktning mot fysikalisk kemi
Publikations- och innehållstyp
- ref (ämneskategori)
- art (ämneskategori)
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