scholarly journals Redox-Active 1D Coordination Polymers of Iron–Sulfur Clusters

2019 ◽  
Vol 141 (9) ◽  
pp. 3940-3951 ◽  
Author(s):  
Noah E. Horwitz ◽  
Jiaze Xie ◽  
Alexander S. Filatov ◽  
Robert J. Papoular ◽  
William E. Shepard ◽  
...  
Keyword(s):  
Coordination Polymers ◽  
Iron Sulfur Clusters ◽  
Iron Sulfur ◽  
Redox Active

scholarly journals Steric and Electronic Effects of Ligand Substitution on Redox-Active Fe4S4-Based Coordination Polymers

2021 ◽  
Author(s):  
Omar Salinas ◽  
Jiaze Xie ◽  
Robert J. Papoular ◽  
Noah E. Horwitz ◽  
Erik Elkaim ◽  
...  
Keyword(s):  
Coordination Polymers ◽  
Photoelectron Spectroscopy ◽  
Electronic Effects ◽  
Iron Sulfur Clusters ◽  
Iron Sulfur ◽  
Redox Active ◽  
Metal Organic ◽  
Uv Visible ◽  
And Function ◽  
Fine Tune

<div>One of the notable advantages of molecular materials is the ability to precisely tune structure, properties, and function via molecular substitutions. While many studies have demonstrated this principle with classic carboxylate‐based coordination polymers, there are comparatively fewer examples where systematic changes to sulfur‐based coordination polymers have been investigated. Here we present such a study on 1D coordination chains of redox‐active</div><div>iron-sulfur clusters linked by methylated 1,4‐benzene‐dithiolates. A series of new iron-sulfur based coordination polymers were synthesized with either 2,5‐dimethyl‐1,4‐benzenedithiol (DMBDT) or 2,3,5,6‐tetramethyl‐1,4‐benzenedithiol. The structures of these compounds have been characterized based on synchrotron Xray</div><div>powder diffraction while their chemical and physical properties have been characterized by techniques including X‐ray photoelectron spectroscopy, cyclic voltammetry and UV–visible spectroscopy. Methylation results in the general trend of increasing electron‐richness in the series, but the tetramethyl version exhibits unexpected properties arising from steric constraints. All these results highlight how substitutions on organic linkers can modulate electronic factors to fine‐tune the electronic structures of metal‐organic materials.</div>

scholarly journals Steric and Electronic Effects of Ligand Substitution on Redox-Active Fe4S4-Based Coordination Polymers

2021 ◽  
Author(s):  
Omar Salinas ◽  
Jiaze Xie ◽  
Robert J. Papoular ◽  
Noah E. Horwitz ◽  
Erik Elkaim ◽  
...  
Keyword(s):  
Coordination Polymers ◽  
Photoelectron Spectroscopy ◽  
Electronic Effects ◽  
Iron Sulfur Clusters ◽  
Iron Sulfur ◽  
Redox Active ◽  
Metal Organic ◽  
Uv Visible ◽  
And Function ◽  
Fine Tune

<div>One of the notable advantages of molecular materials is the ability to precisely tune structure, properties, and function via molecular substitutions. While many studies have demonstrated this principle with classic carboxylate‐based coordination polymers, there are comparatively fewer examples where systematic changes to sulfur‐based coordination polymers have been investigated. Here we present such a study on 1D coordination chains of redox‐active</div><div>iron-sulfur clusters linked by methylated 1,4‐benzene‐dithiolates. A series of new iron-sulfur based coordination polymers were synthesized with either 2,5‐dimethyl‐1,4‐benzenedithiol (DMBDT) or 2,3,5,6‐tetramethyl‐1,4‐benzenedithiol. The structures of these compounds have been characterized based on synchrotron Xray</div><div>powder diffraction while their chemical and physical properties have been characterized by techniques including X‐ray photoelectron spectroscopy, cyclic voltammetry and UV–visible spectroscopy. Methylation results in the general trend of increasing electron‐richness in the series, but the tetramethyl version exhibits unexpected properties arising from steric constraints. All these results highlight how substitutions on organic linkers can modulate electronic factors to fine‐tune the electronic structures of metal‐organic materials.</div>

scholarly journals Biogenesis of Iron–Sulfur Clusters and Their Role in DNA Metabolism

2021 ◽  
Vol 9 ◽  
Author(s):  
Ruifeng Shi ◽  
Wenya Hou ◽  
Zhao-Qi Wang ◽  
Xingzhi Xu
Keyword(s):  
Dna Polymerases ◽  
Protein Assembly ◽  
Eukaryotic Cells ◽  
Ribosome Assembly ◽  
Dna Metabolism ◽  
Cellular Functions ◽  
Active Protein ◽  
Iron Sulfur Clusters ◽  
Iron Sulfur ◽  
Redox Active

Iron–sulfur (Fe/S) clusters (ISCs) are redox-active protein cofactors that their synthesis, transfer, and insertion into target proteins require many components. Mitochondrial ISC assembly is the foundation of all cellular ISCs in eukaryotic cells. The mitochondrial ISC cooperates with the cytosolic Fe/S protein assembly (CIA) systems to accomplish the cytosolic and nuclear Fe/S clusters maturation. ISCs are needed for diverse cellular functions, including nitrogen fixation, oxidative phosphorylation, mitochondrial respiratory pathways, and ribosome assembly. Recent research advances have confirmed the existence of different ISCs in enzymes that regulate DNA metabolism, including helicases, nucleases, primases, DNA polymerases, and glycosylases. Here we outline the synthesis of mitochondrial, cytosolic and nuclear ISCs and highlight their functions in DNA metabolism.

scholarly journals Energy storage inspired by nature – ionic liquid iron–sulfur clusters as electrolytes for redox flow batteries

2019 ◽  
Vol 48 (6) ◽  
pp. 1941-1946 ◽  
Author(s):  
Christian Modrzynski ◽  
Peter Burger
Keyword(s):  
Ionic Liquid ◽  
Ionic Liquids ◽  
High Energy ◽  
High Energy Density ◽  
Redox Flow Battery ◽  
Iron Sulfur Clusters ◽  
Redox Flow Batteries ◽  
Iron Sulfur ◽  
Redox Active ◽  
Battery Electrolyte

A redox flow battery electrolyte with a high energy density based on redox-active ionic liquids with iron–sulfur-clusters was prepared and investigated.

scholarly journals Synthetic Models for Nickel–Iron Hydrogenase Featuring Redox-Active Ligands

2017 ◽  
Vol 70 (5) ◽  
pp. 505 ◽  
Author(s):  
David Schilter ◽  
Danielle L. Gray ◽  
Amy L. Fuller ◽  
Thomas B. Rauchfuss
Keyword(s):  
Active Sites ◽  
Iron Sulfur Clusters ◽  
Nickel Iron Hydrogenase ◽  
Nickel Iron ◽  
Redox States ◽  
Iron Sulfur ◽  
Proton Relay ◽  
Redox Active ◽  
Iron Hydrogenase ◽  
Synthetic Models

The nickel–iron hydrogenase enzymes efficiently and reversibly interconvert protons, electrons, and dihydrogen. These redox proteins feature iron–sulfur clusters that relay electrons to and from their active sites. Reported here are synthetic models for nickel–iron hydrogenase featuring redox-active auxiliaries that mimic the iron–sulfur cofactors. The complexes prepared are NiII(μ-H)FeIIFeII species of formula [(diphosphine)Ni(dithiolate)(μ-H)Fe(CO)2(ferrocenylphosphine)]+ or NiIIFeIFeII complexes [(diphosphine)Ni(dithiolate)Fe(CO)2(ferrocenylphosphine)]+ (diphosphine = Ph2P(CH2)2PPh2 or Cy2P(CH2)2PCy2; dithiolate = –S(CH2)3S–; ferrocenylphosphine = diphenylphosphinoferrocene, diphenylphosphinomethyl(nonamethylferrocene) or 1,1′-bis(diphenylphosphino)ferrocene). The hydride species is a catalyst for hydrogen evolution, while the latter hydride-free complexes can exist in four redox states – a feature made possible by the incorporation of the ferrocenyl groups. Mixed-valent complexes of 1,1′-bis(diphenylphosphino)ferrocene have one of the phosphine groups unbound, with these species representing advanced structural models with both a redox-active moiety (the ferrocene group) and a potential proton relay (the free phosphine) proximal to a nickel–iron dithiolate.

scholarly journals Fe-S cofactors in the SARS-CoV-2 RNA-dependent RNA polymerase are potential antiviral targets

Science ◽  
2021 ◽  
pp. eabi5224
Author(s):  
Nunziata Maio ◽  
Bernard A. P. Lafont ◽  
Debangsu Sil ◽  
Yan Li ◽  
J. Martin Bollinger ◽  
...  
Keyword(s):  
Rna Polymerase ◽  
Metal Binding ◽  
Rna Dependent Rna Polymerase ◽  
Iron Sulfur Clusters ◽  
Metal Binding Sites ◽  
Iron Sulfur ◽  
Cryo Electron Microscopy ◽  
Metal Cofactors ◽  
Antiviral Targets ◽  
Viral Helicase

Severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2), the causal agent of coronavirus disease 2019 (COVID-19), uses an RNA-dependent RNA polymerase (RdRp) for the replication of its genome and the transcription of its genes. We found that the catalytic subunit of the RdRp, nsp12, ligates two iron-sulfur metal cofactors in sites that were modeled as zinc centers in the available cryo-electron microscopy structures of the RdRp complex. These metal binding sites are essential for replication and for interaction with the viral helicase. Oxidation of the clusters by the stable nitroxide TEMPOL caused their disassembly, potently inhibited the RdRp, and blocked SARS-CoV-2 replication in cell culture. These iron-sulfur clusters thus serve as cofactors for the SARS-CoV-2 RdRp and are targets for therapy of COVID-19.

EPR-derived structures of flavin radical and iron-sulfur clusters from Methylosinus sporium 5 reductase

2021 ◽  
Author(s):  
Han Sol Jeong ◽  
Sugyeong Hong ◽  
Hee Seon Yoo ◽  
Jin Kim ◽  
Yujeong Kim ◽  
...  
Keyword(s):  
Carbon Cycle ◽  
Crucial Role ◽  
Methane Monooxygenase ◽  
Global Carbon Cycle ◽  
Ambient Conditions ◽  
Iron Sulfur Clusters ◽  
Iron Sulfur ◽  
Greenhouse Effects ◽  
Global Carbon ◽  
Significant Attention

Methane monooxygenase (MMO) has attracted significant attention owing to its crucial role in the global carbon cycle; it impedes greenhouse effects by converting methane to methanol under ambient conditions. The...

Fine Tunable, Redox Active Octapalladium Chains Supported by Linear Tetraphosphines, Leading to Dynamically 1D Self‐Assembled Coordination Polymers

2021 ◽  
Author(s):  
Tomoaki Tanase ◽  
Kanako Nakamae ◽  
Haruka Miyano ◽  
Yasuyuki Ura ◽  
Yasutaka Kitagawa ◽  
...  
Keyword(s):  
Coordination Polymers ◽  
Redox Active ◽  
Self Assembled
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