Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
Publication date: 18th July 2023
Organic photocatalysts (OPC) are promising materials to enable an energy transition to renewable fuels produced by sunlight, such as green hydrogen, thanks to their low cost, Earth-abundance and processability. State-of-the-art organic photovoltaic (OPV) materials have recently been shown to also act as efficient hydrogen-evolution photocatalysts when used in nanoparticle form. While OPV materials have been extensively investigated by optical and electron spin resonance (ESR) spectroscopies, showing the crucial role that paramagnetic states play in the photovoltaic process,1,2 the details of the photophysical mechanisms leading to catalytic hydrogen generation in these organic semiconductor nanoparticles in aqueous media are largely unexplored. An improved understanding of the mechanisms underlying the photoinitiated processes in OPC will enable the rational design of more efficient materials for cost-competitive technologies.3
Here we apply steady-state and time-resolved ESR techniques to a variety of hydrogen-evolution photocatalysts based on organic semiconductor nanoparticles consisting of polymer electron donors blended with small-molecule or polymer electron acceptors.4,5 The different photogenerated paramagnetic states formed upon photoexcitation of these materials, namely triplet excitons, charge-transfer states and separated charges, are identified and quantified, and their dynamics are studied on the μs time scale. The spin polarisation pattern of the triplet and charge-transfer state spectra observed by time-resolved ESR reveals additional details on their formation mechanism. These new results complement previous optical, morphological and photocatalytic studies of these materials, shedding further light into the origin of their different photocatalytic hydrogen evolution activities.
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