Control of the overpotential of a [FeFe] hydrogenase mimic by a synthetic second coordination sphere

Chemical Communications : Chem Comm
Sandra S NurttilaJoost N H Reek

Abstract

Hydrogen as a renewable fuel is viable when produced sustainably via proton reduction catalysis (PRC). Many homogeneous electrocatalysts perform PRC with high rates, but they all require a large overpotential to drive the reaction. Natural hydrogenase enzymes achieve reversible PRC with potentials close to the thermodynamic equilibrium through confinement of the active site in a well-defined protein pocket. Inspired by nature, we report a strategy that relies on the selective encapsulation of a synthetic hydrogenase mimic in a novel supramolecular cage. Catalyst confinement decreases the PRC overpotential by 150 mV, and is proposed to originate from the cationic cage stabilizing anionic reaction intermediates within the catalytic cycle.

References

Mar 19, 2003·Proceedings of the National Academy of Sciences of the United States of America·Marcetta Y DarensbourgIrene P Georgakaki
Feb 11, 2005·Nature·Cédric TardChristopher J Pickett
Apr 14, 2005·Chemical Reviews·Dennis M VriezemaRoeland J M Nolte
Jun 21, 2005·Inorganic Chemistry·Mathieu RazavetMarc Fontecave
Nov 17, 1978·Science·J R Bolton
Sep 12, 2007·Chemical Reviews·Wolfgang LubitzMaurice van Gastel
Oct 12, 2007·Chemical Reviews·Arthur J Esswein, Daniel G Nocera
Dec 18, 2008·Chemical Society Reviews·Frédéric Gloaguen, Thomas B Rauchfuss
Oct 7, 2009·Proceedings of the National Academy of Sciences of the United States of America·Sven T StrippThomas Happe
Apr 2, 2010·Current Opinion in Biotechnology·Bryan E BartonThomas B Rauchfuss
Jun 12, 2010·Journal of the American Chemical Society·Michael L SingletonMarcetta Y Darensbourg
Oct 6, 2010·Angewandte Chemie·Michael J WiesterChad A Mirkin
Aug 17, 2012·Chemical Communications : Chem Comm·Anindya RoyGiovanna Ghirlanda
Jun 28, 2013·Nature·G BerggrenM Fontecave
Mar 25, 2014·Chemical Reviews·Wolfgang LubitzEdward Reijerse
Jul 16, 2014·Journal of the American Chemical Society·Agnieszka Adamska-VenkateshWolfgang Lubitz
Jul 17, 2014·Chemical Society Reviews·Salvatore ZarraJonathan R Nitschke
Oct 24, 2014·Chemical Society Reviews·Stefan H A M LeendersJoost N H Reek
Mar 5, 2015·Journal of the American Chemical Society·Xu JingChunying Duan
Apr 22, 2015·Chemical Reviews·Casey J BrownKenneth N Raymond
Aug 14, 2015·Energy & Environmental Science·Vincent Artero, Jean-Michel Saveant
Dec 21, 2016·Journal of the American Chemical Society·Wolfgang BrennerJonathan R Nitschke
Aug 18, 2018·Chemistry : a European Journal·Sandra S NurttilaJoost N H Reek

❮ Previous
Next ❯

Citations

Jan 28, 2021·Chemical Society Reviews·Jonathan Trouvé, Rafael Gramage-Doria
Jun 26, 2021·Chemical Science·Tom KeijerJoost N H Reek
Jun 25, 2021·Chemical Science·Sonja PullenGuido H Clever
Apr 18, 2020·Journal of the American Chemical Society·Riccardo ZaffaroniJoost N H Reek
Jan 15, 2020·Journal of the American Chemical Society·Rebecca L SpicerPaul J Lusby

❮ 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.