Proton-Coupled Electron Transfer Drives Long-Range Proton Translocation in Bioinspired Systems

Journal of the American Chemical Society
Emmanuel OdellaAna L Moore

Abstract

Proton-coupled electron transfer (PCET) combines the movement of fundamental charged species to form an essential link between electron- and proton-transport reactions in bioenergetics and catalysis in general. The length scale over which proton transport may occur within PCET processes and the thermodynamic consequences of the resulting proton chemical potential to the oxidation reaction driving these PCET processes have not been generally established. Here we report the design of bioinspired molecules that employ oxidation-reduction processes to move reversibly two, three, and four protons via a Grotthuss-type mechanism along hydrogen-bonded networks up to ∼16 Å in length. These molecules are composed of benzimidazole moieties linking a phenol to the final proton acceptor, a cyclohexylimine. Following electrochemical oxidation of the phenol, the appearance of an infrared band at 1660 cm-1 signals proton arrival at the terminal basic site. Switching the electrode potential to reducing conditions reverses the proton translocation and resets the structure to the initial species. In addition to mimicking the first step of the iconic PCET process used by the Tyr z -His190 redox relay in photosystem II to oxidize water, this work s...Continue Reading

References

May 17, 2000·Biochimica Et Biophysica Acta·C Tommos, G T Babcock
Jan 24, 2008·Proceedings of the National Academy of Sciences of the United States of America·Todd F MarkleJames M Mayer
Apr 7, 2009·Annual Review of Biochemistry·Steven Y Reece, Daniel G Nocera
Nov 6, 2010·Chemical Reviews·Sharon Hammes-Schiffer, Alexei A Stuchebrukhov
Nov 19, 2010·Chemical Reviews·Jillian L DempseyHarry B Gray
Oct 28, 2011·Accounts of Chemical Research·Julien BoninCédric Tard
Apr 2, 2014·Chemical Reviews·Agostino MiglioreDavid N Beratan
Apr 2, 2015·Annual Review of Physical Chemistry·Dongping Zhong
Jan 9, 2018·Accounts of Chemical Research·S Jimena MoraAna L Moore
May 13, 2018·Proceedings of the National Academy of Sciences of the United States of America·Zhanjun GuoBridgette A Barry
Nov 1, 2018·Journal of the American Chemical Society·Emmanuel OdellaAna L Moore

❮ Previous
Next ❯

Citations

Aug 14, 2020·Physical Chemistry Chemical Physics : PCCP·James B DerrValentine I Vullev
Jan 13, 2021·Photosynthesis Research·Emmanuel OdellaAna L Moore
Feb 20, 2021·Journal of the American Chemical Society·Yusuke YonedaGraham R Fleming
Jul 3, 2021·Frontiers in Chemistry·Divya KaurM R Gunner
Jul 27, 2021·The Journal of Physical Chemistry. a·Zong-Ying LiuPi-Tai Chou
Aug 12, 2021·Journal of the American Chemical Society·Hannah SayreRobert R Knowles
Dec 19, 2020·Journal of the American Chemical Society·Walter D GuerraAna L Moore
Nov 27, 2020·The Journal of Physical Chemistry. B·Ananta DeyHirendra N Ghosh
Jan 7, 2021·Journal of the American Chemical Society·Robin TyburskiLeif Hammarström
Oct 30, 2021·The Journal of Physical Chemistry. B·Dmitry V Matyushov, Marshall D Newton

❮ 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.