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dc.contributor.authorDana, Jayanta
dc.contributor.authorKhan, Ramsha
dc.contributor.authorWeckman, Timo
dc.contributor.authorHonkala, Karoliina
dc.contributor.authorTkachenko, Nikolai V.
dc.date.accessioned2023-11-13T10:01:25Z
dc.date.available2023-11-13T10:01:25Z
dc.date.issued2023
dc.identifier.citationDana, J., Khan, R., Weckman, T., Honkala, K., & Tkachenko, N. V. (2023). Laterally Bound Co Porphyrin on CdTe QD : A Long-Lived Charge-Separated Nanocomposite. <i>Journal of Physical Chemistry C</i>, <i>127</i>(21), 10164-10173. <a href="https://doi.org/10.1021/acs.jpcc.3c00856" target="_blank">https://doi.org/10.1021/acs.jpcc.3c00856</a>
dc.identifier.otherCONVID_183351247
dc.identifier.urihttps://jyx.jyu.fi/handle/123456789/91903
dc.description.abstractCobalt porphyrin (CoP) derivatives are potential compounds for photocatalytic CO2 reduction which must be activated by photoinduced electron transfer from a suitable electron donor. Herein, we have prepared and studied the photophysics of CdTe quantum dots (CQD) coupled with CoP derivatives where CQDs act as the light antenna and the electron donor and CoP acts as the electron acceptor. To facilitate the nanocomposite formation of CoP with CQD, CoP has been equipped with a −COOH anchoring group which leads to strong complexation between CQD and CoP as observed in the absorption spectra by a gradual shift in the Soret absorption band. This is attributed to the lateral binding geometry of CoP through the −COOH anchoring group and Co-center coordination to CQD, which helps to bring CoP close to the CQD. Our DFT calculations have identified that this lateral geometry is more favorable than the upright orientation on the CdTe (110) surface. The redox levels have been determined from cyclic voltammetry which shows that the electron transfer (ET) from CQD to CoP is feasible. The strong luminescence quenching of CQD in the presence of CoP has also suggested quantitative CQD/CoP nanocomposite formation and pointed to the ET from QDs to CoP. The charge carrier dynamics have been monitored using femtosecond transient absorption (TA) spectroscopy. The TA spectral analysis has shown efficient ET in CQD/CoP which proves that our 4 nm CQD acts as an efficient electron donor for the CoP counterpart. The CQD excited state lifetime is shortened along with delayed Soret band bleaching of CoP in this nanocomposite. From the global fitting of TA data, the estimated average ET time constant from CQD to a CoP molecule is approximately 70 ps, and the charge recombination time is ≫5 ns. Also, differences in the TA spectra after ET have been observed which can be associated with the changes in the binding geometry of CoP on the CQD surface, which is lateral in the case of the ground-state complex to the upright orientation after the ET process. Hence, the studied CQD/CoP nanocomposites are promising materials to initiate CO2 reduction through photoexcitation of the CQD that activates the CoP molecular catalyst through the ET.en
dc.format.mimetypeapplication/pdf
dc.language.isoeng
dc.publisherAmerican Chemical Society
dc.relation.ispartofseriesJournal of Physical Chemistry C
dc.rightsIn Copyright
dc.titleLaterally Bound Co Porphyrin on CdTe QD : A Long-Lived Charge-Separated Nanocomposite
dc.typearticle
dc.identifier.urnURN:NBN:fi:jyu-202311137927
dc.contributor.laitosKemian laitosfi
dc.contributor.laitosDepartment of Chemistryen
dc.contributor.oppiaineFysikaalinen kemiafi
dc.contributor.oppiaineNanoscience Centerfi
dc.contributor.oppiainePhysical Chemistryen
dc.contributor.oppiaineNanoscience Centeren
dc.type.urihttp://purl.org/eprint/type/JournalArticle
dc.type.coarhttp://purl.org/coar/resource_type/c_2df8fbb1
dc.description.reviewstatuspeerReviewed
dc.format.pagerange10164-10173
dc.relation.issn1932-7447
dc.relation.numberinseries21
dc.relation.volume127
dc.type.versionacceptedVersion
dc.rights.copyright© 2023 American Chemical Society
dc.rights.accesslevelopenAccessfi
dc.relation.grantnumber5482-2a4a9
dc.subject.ysoheterosykliset yhdisteet
dc.subject.ysokatalyytit
dc.subject.ysopelkistys
dc.subject.ysohiilidioksidin talteenotto ja varastointi
dc.subject.ysokoboltti
dc.subject.ysofotokatalyysi
dc.subject.ysonanorakenteet
dc.format.contentfulltext
jyx.subject.urihttp://www.yso.fi/onto/yso/p38837
jyx.subject.urihttp://www.yso.fi/onto/yso/p15480
jyx.subject.urihttp://www.yso.fi/onto/yso/p9117
jyx.subject.urihttp://www.yso.fi/onto/yso/p24009
jyx.subject.urihttp://www.yso.fi/onto/yso/p15221
jyx.subject.urihttp://www.yso.fi/onto/yso/p38243
jyx.subject.urihttp://www.yso.fi/onto/yso/p25315
dc.rights.urlhttp://rightsstatements.org/page/InC/1.0/?language=en
dc.relation.doi10.1021/acs.jpcc.3c00856
dc.relation.funderJane and Aatos Erkko Foundationen
dc.relation.funderJane ja Aatos Erkon säätiöfi
jyx.fundingprogramFoundationen
jyx.fundingprogramSäätiöfi
jyx.fundinginformationThis project was supported by the Jane & Aatos Erkko Foundation (JAES/LACOR-31228007701).
dc.type.okmA1


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