Recovery of Active and Efficient Photocatalytic H2 Production for CdSe Quantum Dots

Burke, Rebeckah; Cogan, Nicole M.  Briglio; Oi, Aidan; Krauss, Todd D.

doi:10.1021/acs.jpcc.8b01237

Title: Recovery of Active and Efficient Photocatalytic H₂ Production for CdSe Quantum Dots

Journal Article · Mon May 07 00:00:00 EDT 2018 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b01237· OSTI ID:1436089

Burke, Rebeckah ^[1]; Cogan, Nicole M. Briglio ^[1]; Oi, Aidan ^[1]; Krauss, Todd D. ^[2]

Univ. of Rochester, NY (United States). Dept. of Chemistry
Univ. of Rochester, NY (United States). Dept. of Chemistry and Inst. of Optics

Recently, colloidal semiconductor quantum dots (QDs) have shown great promise as photocatalysts for the production of chemical fuels by sunlight. Here, the efficiency of photocatalytic hydrogen (H₂) production for integrated systems of large diameter (4.4 nm) CdSe QDs as light harvesting nanoparticles with varying concentrations of nickel-dihydrolipoic acid (Ni-DHLA) small molecule catalysts was measured. While exhibiting excellent robustness and longevity, the efficiency of H₂ production for equimolar catalyst and QDs was relatively poor. However, the efficiency was found to increase substantially with increasing Ni-DHLA:QD molar ratios Surprisingly, this high activity was only observed with the use of 3-mercaptopropionic acid (MPA) ligands, while CdSe QDs capped with dihydrolipoic acid (DHLA) exhibited poor performance in comparison, indicating that the QD capping ligand has a substantial impact on the catalytic performance. Finally, ultrafast transient absorption spectroscopic measurements of the electron transfer (ET) dynamics show fast ET to the catalyst. Importantly, an increase in ET efficiency is observed as the catalyst concentration is increased. Together, these results suggest that for these large QDs, tailoring the QD surface environment for facile ET and increasing catalyst concentrations increases the probability of ET from QDs to Ni-DHLA, overcoming the relatively small driving force for ET and decreased surface electron density for large diameter QDs.

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Research Organization:: Univ. of Rochester, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: SC0002106; FG02-09ER16121

OSTI ID:: 1436089

Journal Information:: Journal of Physical Chemistry. C, Vol. 122, Issue 25; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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