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Photocatalytic H-2 production using a hybrid assembly of an [FeFe]-hydrogenase model and CdSe quantum dot linked through a thiolato-functionalized cyclodextrin
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2017 (English)In: Faraday discussions (Online), ISSN 1359-6640, E-ISSN 1364-5498, Vol. 198, 197-209 p.Article in journal (Refereed) Published
Abstract [en]

It is a great challenge to develop iron-based highly-efficient and durable catalytic systems for the hydrogen evolution reaction (HER) by understanding and learning from [FeFe]-hydrogenases. Here we report photocatalytic H-2 production by a hybrid assembly of a sulfonate-functionalized [FeFe]-hydrogenase mimic (1) and CdSe quantum dot (QD), which is denoted as 1/beta-CD-6-S-CdSe (beta-CD-6-SH = 6-mercapto-beta-cyclodextrin). In this assembly, thiolato-functionalized beta-CD acts not only as a stabilizing reagent of CdSe QDs but also as a host compound for the diiron catalyst, so as to confine CdSe QDs to the space near the site of diiron catalyst. In addition, another two reference systems comprising MAA-CdSe QDs (HMAA = mercaptoacetic acid) and 1 in the presence and absence of beta-CD, denoted as 1/beta-CD/MAA-CdSe and 1/MAA-CdSe, were studied for photocatalytic H-2 evolution. The influences of beta-CD and the stabilizing reagent beta-CD-6-S- on the stability of diiron catalyst, the fluorescence lifetime of CdSe QDs, the apparent electron transfer rate, and the photocatalytic H-2-evolving efficiency were explored by comparative studies of the three hybrid systems. The 1/beta-CD-6-SCdSe system displayed a faster apparent rate for electron transfer from CdSe QDs to the diiron catalyst compared to that observed for MAA-CdSe-based systems. The total TON for visible-light driven H-2 evolution by the 1/beta-CD-6-S-CdSe QDs in water at pH 4.5 is about 2370, corresponding to a TOF of 150 h(-1) in the initial 10 h of illumination, which is 2.7- and 6.6-fold more than the amount of H-2 produced from the reference systems 1/beta-CD/MAA-CdSe and 1/MAA-CdSe. Additionally, 1/beta-CD-6-S-CdSe gave 2.4-5.1 fold enhancement in the apparent quantum yield and significantly improved the stability of the system for photocatalytic H-2 evolution.

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2017. Vol. 198, 197-209 p.
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-210432DOI: 10.1039/c6fd00207bISI: 000402870300012PubMedID: 28267170OAI: oai:DiVA.org:kth-210432DiVA: diva2:1119172
Funder
Knut and Alice Wallenberg Foundation
Note

QC 20170703

Available from: 2017-07-03 Created: 2017-07-03 Last updated: 2017-07-03Bibliographically approved

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