Mechanistic Insights into the Photocatalytic Hydrogen Production of Y5 and Y6 Nanoparticles

Utilization of solarenergy in organic semiconductorsrelies oncomplicated photophysical processes due to the strong electron-holeinteractions. To gain a better understanding of these processes andtheir effect on the photocatalytic performance of non-fullerene acceptors(NFAs) within nanoparticles (NPs), we compared the excited-state dynamicsand photocatalytic hydrogen production activity of two NFA-based NPs,Y5 and Y6. Our results show that under LED light irradiation, Y5 NPsexhibit 14 times better hydrogen production activity than Y6 NPs.The hydrogen production activity was also evaluated under Xenon lightirradiation (AM1.5G, 100 mW & BULL;cm(-2)) for Y5 NPs,yielding 410 mmol/g after 24 h. Time-resolved spectroscopy experimentsrevealed a longer triplet lifetime for Y5 compared to Y6 NPs, andthe lifetime was reduced upon addition of the electron donor ascorbate.This suggests the involvement of the triplet state in reductive quenchingand better hydrogen evolution reaction performance for Y5 NPs. Thegood agreement between fluorescence and triplet lifetimes observedfor Y5 NPs was attributed to reverse intersystem crossing, which repopulatesthe excited singlet state through thermally activated delayed fluorescence(TADF). The absence of TADF in Y6 NPs could limit its efficiency forhydrogen evolution reaction, in addition to the intrinsically shortertriplet lifetime and reduction potential difference, making it animportant factor to consider in Y series-based NPs.

Hammarström, Leif,1964-Uppsala universitet,Fysikalisk kemi(Swepub:uu)leifhamm (författare)
Tian, Haining,1983-Uppsala universitet,Fysikalisk kemi(Swepub:uu)haiti806 (författare)
Uppsala universitetFysikalisk kemi (creator_code:org_t)

Ingår i:The Journal of Physical Chemistry C: American Chemical Society (ACS)127:26, s. 12631-126391932-74471932-7455

Av författaren/redakt...: Brnovic, Andjela; Hammarström, Lei ...; Tian, Haining, 1 ...

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