화학공학소재연구정보센터
Journal of the American Chemical Society, Vol.140, No.32, 10117-10120, 2018
Electron Transfer into Electron-Accumulated Nanocrystals: Mimicking Intermediate Events in Multielectron Photocatalysis II
The overall efficiency of multielectron photocatalytic reactions is, often much lower than the charge-separation yield reported for the first charge transfer (CT) event. Our recent study has partially linked this gap to CT from charge-accumulated light harvesters. Another possible intermediate event lowering the efficiency is CT into charge-accumulated nanocatalysts. To study this event, we built a "toy" system using nanocrystal quantum dots (QDs) doped with extra electrons to mimick charge-accumulated nanocatalysts. We measured electron transfer (ET) from photoexcited molecular light harvesters into doped QDs using transient absorption spectroscopy. The measurements reveal that the pre-existing electron slows down ET from 37.8 +/- 2.2 ps in the neutral sample to 93.4 +/- 8.6 ps in the singly doped sample, accelerates charge recombination (CR) from 7.02 +/- 0.84 to 3.69 +/- 0.25 ns, and lowers the electron-injection yield by similar to 14%. This study uncovers yet another possible intermediate event lowering the efficiency of multielectron photocatalysis.