Straightforward computational determination of energy-transfer kinetics through the application of the Marcus theory

Solé-Daura, Albert; Maseras, Feliu

doi:10.1039/d4sc03352c

Chem. Sci.

2024

DOI: 10.1039/d4sc03352c

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Straightforward computational determination of energy-transfer kinetics through the application of the Marcus theory

Albert Solé-Daura,

Feliu Maseras

Abstract: Energy transfer (EnT) photocatalysis holds the potential to revolutionize synthetic chemistry, unlocking the excited-state reactivity of non-chromophoric compounds via indirect sensitization. This strategy gives access to synthetic routes to valuable...

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Cited by 3 publications

References 60 publications

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Triplet‐Sensitized Switching of High‐Energy‐Density Norbornadienes for Molecular Solar Thermal Energy Storage with Visible Light

Zähringer,

Perez Lopez,

Schulte

et al. 2024

Angewandte Chemie

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Norbornadiene‐based photoswitches have emerged as promising candidates for harnessing and storing solar energy, holding great promise as a viable solution to meet the growing energy demands. Despite their potential, the effectiveness of their direct photochemical conversion into the resulting quadricyclanes has room for improvement owing to (i) moderate quantum yields, (ii) poor overlap with the solar spectrum and (iii) photochemical back reactions. Herein, we present an approach to enhance the performance of such molecular solar thermal energy storage (MOST) systems through the triplet‐sensitized conversion of aryl‐substituted norbornadienes. Our study combines deep spectroscopic analyses, irradiation experiments, and quantum mechanical calculations to elucidate the energy transfer mechanism and inherent advantages of the resulting MOST systems. We demonstrate remarkable quantum yields using readily available sensitizers under both LED and solar light irradiation, significantly surpassing those achieved through direct excitation with photons of higher energy. In contrast to the conventional approach, light‐induced back reactions of the high‐energy products do not play any role, allowing quantitative switching within minutes. These results not only underscore the potential of triplet‐sensitized MOST systems to leverage the high energy storage capabilities of multistate photoswitches but they might also stimulate the broader usage of sensitization strategies in photochemical energy conversion.

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Triplet‐Sensitized Switching of High‐Energy‐Density Norbornadienes for Molecular Solar Thermal Energy Storage with Visible Light

Zähringer,

Perez Lopez,

Schulte

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Triplet‐Sensitized Switching of High‐Energy‐Density Norbornadienes for Molecular Solar Thermal Energy Storage with Visible Light

Zähringer,

Perez Lopez,

Schulte

et al. 2024

Angew Chem Int Ed

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Visible Light-Induced Regioselective E to Z Isomerization of Polarized 1,3-Dienes: Experimental and Theoretical Insights

Saha,

Banerjee,

Malo

et al. 2024

J. Org. Chem.

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The stereocontrol of E → Z isomerization on a (1E,3E)-diene, instead of a simple alkene, can be more challenging due to the increased number of isomerization possibilities. Herein, we report visible light-mediated regioselective (1E,3E → 1E,3Z) isomerization of (1E,3E)-diene. The reaction conditions are mild and easy to apply and can be applied to a wide range of substances, with an excellent yield and selectivity (90:10). It is evident from the crystal structures that the cause of regioselectivity for the isomerization of 1,3-diene may not be limited to 1,3-allylic strains; CH−π interaction may also play a vital role. Computational studies suggest that this regioselective photoisomerization is a thermodynamically feasible process and requires the accumulation of spin density on the modified double bond for the transformation to occur.

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Straightforward computational determination of energy-transfer kinetics through the application of the Marcus theory

Abstract: Energy transfer (EnT) photocatalysis holds the potential to revolutionize synthetic chemistry, unlocking the excited-state reactivity of non-chromophoric compounds via indirect sensitization. This strategy gives access to synthetic routes to valuable...

Cited by 3 publications

References 60 publications

Triplet‐Sensitized Switching of High‐Energy‐Density Norbornadienes for Molecular Solar Thermal Energy Storage with Visible Light

Triplet‐Sensitized Switching of High‐Energy‐Density Norbornadienes for Molecular Solar Thermal Energy Storage with Visible Light

Triplet‐Sensitized Switching of High‐Energy‐Density Norbornadienes for Molecular Solar Thermal Energy Storage with Visible Light

Visible Light-Induced Regioselective E to Z Isomerization of Polarized 1,3-Dienes: Experimental and Theoretical Insights

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