Ultrafast photodriven intramolecular electron transfer from an iridium-based water-oxidation catalyst to perylene diimide derivatives.

Proceedings of the National Academy of Sciences of the United States of America
Michael T VagniniMichael R Wasielewski

Abstract

Photodriving the activity of water-oxidation catalysts is a critical step toward generating fuel from sunlight. The design of a system with optimal energetics and kinetics requires a mechanistic understanding of the single-electron transfer events in catalyst activation. To this end, we report here the synthesis and photophysical characterization of two covalently bound chromophore-catalyst electron transfer dyads, in which the dyes are derivatives of the strong photooxidant perylene-3,4:9,10-bis(dicarboximide) (PDI) and the molecular catalyst is the Cp*Ir(ppy)Cl metal complex, where ppy = 2-phenylpyridine. Photoexcitation of the PDI in each dyad results in reduction of the chromophore to PDI(•-) in less than 10 ps, a process that outcompetes any generation of (3*)PDI by spin-orbit-induced intersystem crossing. Biexponential charge recombination largely to the PDI-Ir(III) ground state is suggestive of multiple populations of the PDI(•-)-Ir(IV) ion-pair, whose relative abundance varies with solvent polarity. Electrochemical studies of the dyads show strong irreversible oxidation current similar to that seen for model catalysts, indicating that the catalytic integrity of the metal complex is maintained upon attachment to the high...Continue Reading

References

Aug 9, 2002·Journal of the American Chemical Society·Tamar van der BoomMichael R Wasielewski
Mar 18, 2004·Chemical Society Reviews·Frank WürthnerChantu R Saha-Möller
Jan 15, 2005·Optics Letters·Hanju Rhee, Taiha Joo
Mar 2, 2005·Proceedings of the National Academy of Sciences of the United States of America·Randall H GoldsmithMichael R Wasielewski
Sep 27, 2005·Inorganic Chemistry·James H Alstrum-AcevedoThomas J Meyer
Jul 3, 2007·The Journal of Organic Chemistry·Paramasivan RajasinghBoris Rybtchinski
Feb 14, 2008·Journal of the American Chemical Society·Aaron A RachfordFelix N Castellano
Feb 27, 2008·The Journal of Physical Chemistry. a·Jovan M GiaimoMichael R Wasielewski
Dec 10, 2008·Optics Express·Chul Hoon Kim, Taiha Joo
Apr 21, 2009·The Journal of Physical Chemistry. a·Evgeny O DanilovFelix N Castellano
Jun 6, 2009·Journal of the American Chemical Society·Jonathan F HullRobert H Crabtree
Aug 8, 2009·Chemical Communications : Chem Comm·Rubén D CostaAngela Sastre-Santos
Nov 12, 2009·Accounts of Chemical Research·Devens GustAna L Moore
Jan 22, 2010·The Journal of Physical Chemistry. B·V SivamuruganS Valiyaveettil
Jun 12, 2010·Journal of the American Chemical Society·Amanda P S SamuelMichael R Wasielewski
Oct 23, 2010·Journal of the American Chemical Society·James D BlakemoreRobert H Crabtree
Nov 26, 2010·Journal of the American Chemical Society·Zuofeng ChenThomas J Meyer
May 24, 2011·The Journal of Physical Chemistry. B·Victoria L GundersonMichael R Wasielewski
Jun 16, 2011·Journal of the American Chemical Society·Nathan D SchleyGary W Brudvig

❮ Previous
Next ❯

Citations

Jul 20, 2012·Inorganic Chemistry·Valentina PrusakovaFelix N Castellano
Jul 5, 2013·Journal of the American Chemical Society·Ulrich HintermairRobert H Crabtree
Mar 20, 2013·The Journal of Organic Chemistry·Anna G SlaterNeil R Champness
Jun 14, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Felix N Castellano
Sep 29, 2012·Proceedings of the National Academy of Sciences of the United States of America·Javier J ConcepcionThomas J Meyer
Aug 14, 2015·Chemical Reviews·Frank WürthnerDavid Schmidt
Nov 12, 2015·The Journal of Physical Chemistry Letters·M Kyle BrennamanThomas J Meyer
Oct 30, 2015·Chemical Reviews·Dennis L AshfordThomas J Meyer
Jan 27, 2015·Current Opinion in Chemical Biology·Andreas Bachmeier, Fraser Armstrong
May 19, 2017·Physical Chemistry Chemical Physics : PCCP·Francesco NastasiMaurizio Prato
Nov 20, 2014·Chemical Communications : Chem Comm·Valentin KunzFrank Würthner
Jun 15, 2017·Journal of the American Chemical Society·Ting JiangMichael J Therien
Jul 14, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Benjamin R ReinerCasey R Wade
Oct 14, 2017·Physical Chemistry Chemical Physics : PCCP·Shinaj K RajagopalMahesh Hariharan
Aug 19, 2016·Dalton Transactions : an International Journal of Inorganic Chemistry·Federico RonconiSebastiano Campagna
May 28, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Ross J DavidsonPaul J Low
May 16, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Julianne M ThomsenGary W Brudvig
Dec 17, 2014·Angewandte Chemie·Marcus SchulzeFrank Würthner
Mar 8, 2019·Chemical Communications : Chem Comm·Chi Lun LeeChi-Ming Che
Oct 20, 2012·Chemical Society Reviews·John R Swierk, Thomas E Mallouk
Jul 20, 2019·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Agnese AmatiFrank Würthner
Jun 12, 2013·Chemistry : a European Journal·Channa A WijesingheFrancis D'Souza
Jul 31, 2014·Organic & Biomolecular Chemistry·Mario MarciaAndreas Hirsch
Jun 20, 2013·Organic & Biomolecular Chemistry·Flynt S GoodsonSourav Saha
Aug 21, 2014·Organic & Biomolecular Chemistry·C SenterCharles L Liotta
May 26, 2021·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Jasper DeckersWouter Maes
Mar 20, 2018·Journal of the American Chemical Society·Peter W MünichDirk M Guldi
Feb 24, 2015·Inorganic Chemistry·Lei WangLeif Hammarström
Dec 17, 2014·ACS Applied Materials & Interfaces·Janardhan BalapanuruKian Ping Loh
Jun 10, 2014·The Journal of Physical Chemistry. a·Catherine E McCuskerFelix N Castellano

❮ Previous
Next ❯

Related Concepts

Trending Feeds

COVID-19

Coronaviruses encompass a large family of viruses that cause the common cold as well as more serious diseases, such as the ongoing outbreak of coronavirus disease 2019 (COVID-19; formally known as 2019-nCoV). Coronaviruses can spread from animals to humans; symptoms include fever, cough, shortness of breath, and breathing difficulties; in more severe cases, infection can lead to death. This feed covers recent research on COVID-19.

Blastomycosis

Blastomycosis fungal infections spread through inhaling Blastomyces dermatitidis spores. Discover the latest research on blastomycosis fungal infections here.

Nuclear Pore Complex in ALS/FTD

Alterations in nucleocytoplasmic transport, controlled by the nuclear pore complex, may be involved in the pathomechanism underlying multiple neurodegenerative diseases including Amyotrophic Lateral Sclerosis and Frontotemporal Dementia. Here is the latest research on the nuclear pore complex in ALS and FTD.

Applications of Molecular Barcoding

The concept of molecular barcoding is that each original DNA or RNA molecule is attached to a unique sequence barcode. Sequence reads having different barcodes represent different original molecules, while sequence reads having the same barcode are results of PCR duplication from one original molecule. Discover the latest research on molecular barcoding here.

Chronic Fatigue Syndrome

Chronic fatigue syndrome is a disease characterized by unexplained disabling fatigue; the pathology of which is incompletely understood. Discover the latest research on chronic fatigue syndrome here.

Evolution of Pluripotency

Pluripotency refers to the ability of a cell to develop into three primary germ cell layers of the embryo. This feed focuses on the mechanisms that underlie the evolution of pluripotency. Here is the latest research.

Position Effect Variegation

Position Effect Variagation occurs when a gene is inactivated due to its positioning near heterochromatic regions within a chromosome. Discover the latest research on Position Effect Variagation here.

STING Receptor Agonists

Stimulator of IFN genes (STING) are a group of transmembrane proteins that are involved in the induction of type I interferon that is important in the innate immune response. The stimulation of STING has been an active area of research in the treatment of cancer and infectious diseases. Here is the latest research on STING receptor agonists.

Microbicide

Microbicides are products that can be applied to vaginal or rectal mucosal surfaces with the goal of preventing, or at least significantly reducing, the transmission of sexually transmitted infections. Here is the latest research on microbicides.

Related Papers

Journal of the American Chemical Society
Nattawut KaveevivitchaiRandolph P Thummel
Accounts of Chemical Research
Javier J ConcepcionThomas J Meyer
© 2021 Meta ULC. All rights reserved