Publications related to An Iron Carbonyl Pyridonate Complex Related to the Active Site of the [Fe]-Hydrogenase (Hmd)

Stabilizing Unusual Oxidation States of Lanthanides in Molecular Complexes: Synthesis, Properties, and Reactivity

The chemistry of divalent lanthanides has generated increasing interest in the past years due to their redox properties and unique reaction pathways. Notably, molecular complexes of low-valent lanthanides have been shown to be suitable one-electron reducta ...

EPFL2022

Load-bearing hydrogels ionically reinforced through competitive ligand exchanges

Esther Amstad, Mathias Steinacher, Matteo Hirsch, Ran Zhao

Fast advances in soft robotics and tissue engineering demand for new soft materials whose mechanical properties can be interchangeably and locally varied, thereby enabling, for example, the design of soft joints within an integral material. Inspired by nat ...

ROYAL SOC CHEMISTRY2021

Carbon dioxide reduction by lanthanide(iii) complexes supported by redox-active Schiff base ligands

Rosario Scopelliti, Marinella Mazzanti, Davide Toniolo, Nadir Jori

Here we have explored the ability of Schiff bases to act as electron reservoirs and to enable the multi-electron reduction of small molecules by lanthanide complexes. We report the reductive chemistry of the Ln(iii) complexes of the tripodal heptadentate S ...

2020

Delivery of a Masked Uranium(II) by an Oxide-Bridged Diuranium(III) Complex

Marinella Mazzanti, Farzaneh Fadaei Tirani, Dieuwertje Katelijn Modder

Oxide is an attractive linker for building polymetallic complexes that provide molecular models for metal oxide activity, but studies of these systems are limited to metals in high oxidation states. Herein, we synthesized and characterized the molecular an ...

Wiley-VCH Verlag GmbH2021

Accessing the plus IV Oxidation State in Molecular Complexes of Praseodymium

Marinella Mazzanti, Ivica Zivkovic, Farzaneh Fadaei Tirani, Aurélien René Willauer

Out of the 14 lanthanide (Ln) ions, molecular complexes of Ln(IV) were known only for cerium and more recently terbium. Here we demonstrate that the +IV oxidation state is also accessible for the large praseodymium (Pr) cation. The oxidation of the tetraki ...

2020

Structure-Property Relationships of Microphase-Separated Metallosupramolecular Polymers

Emad Oveisi, Stephen Schrettl

The structural, thermomechanical, and viscoelastic properties of metallosupramolecular polymers (MSPs) can be controlled through the choice of the multiligand monomer and the nature of the metal salt from which these materials are assembled. This versatili ...

American Chemical Society2020

High-Valent Nickel Promoted by Atomically Embedded Copper for Efficient Water Oxidation

Jun Li, Bo Zhang, Yun Liu, Ning Wang

Efficient and low-cost electrocatalysts for oxygen evolution reaction (OER), particularly in neutral conditions, are of significant importance for renewable energy technologies such as CO2 reduction and seawater splitting electrolysis. High-valent transiti ...

AMER CHEMICAL SOC2020

Stability profiles of transition metal oxides in the oxygen evolution reaction in alkaline medium

Xile Hu, Aliki Moysiadou

The electrochemical water splitting reaction can convert renewable electricity into clean hydrogen fuel. The efficiency of water splitting is limited to a large extent by the sluggish oxygen evolution reaction (OER). Numerous transition metal oxides have b ...

Royal Society of Chemistry2019

A Functional Model of [Fe]-Hydrogenase

Rosario Scopelliti, Matthew Wodrich, Xile Hu, Simona Mazza, Tao Xu

[Fe]-Hydrogenase catalyzes the hydrogenation of a biological substrate via the heterolytic splitting of molecular hydrogen. While many synthetic models of [Fe]-hydrogenase have been prepared, none yet are capable of activating H-2 on their own. Here, we re ...

American Chemical Society2016

Lanthanide(II) Complexes Supported by N,O-Donor Tripodal Ligands: Synthesis, Structure, and Ligand-Dependent Redox Behavior

Rosario Scopelliti, Marinella Mazzanti, Julie Renée Michelle Andrez

The preparation and characterization of a series of complexes of the Yb and Eu cations in the oxidation state II and III with the tetradentate N,O-donor tripodal ligands (tris(2-pyridylmethyl)amine (TPA), BPA(-) (HBPA=bis(2-pyridylmethyl)(2-hydroxybenzyl)a ...

2015

Reconstitution of [Fe]-hydrogenase using model complexes

Matthew Wodrich, Xile Hu, Dafa Chen, Tao Xu

[Fe]-Hydrogenase catalyses the reversible hydrogenation of a methenyltetrahydromethanopterin substrate, which is an intermediate step during the methanogenesis from CO2 and H-2. The active site contains an iron-guanylylpyridinol cofactor, in which Fe2+ is ...

Nature Publishing Group2015

Mimicking Enzymatic Active Sites on Surfaces for Energy Conversion Chemistry

Klaus Kern, Sebastian Stepanow, Magalí Alejandra Lingenfelder

Metal organic supramolecular chemistry on surfaces has matured to a point where its underlying growth mechanisms are well understood and structures of defined coordination environments of metal atoms can be synthesized in a controlled and reproducible proc ...

Amer Chemical Soc2015

Asymmetric Rhodium(I)-Catalyzed C-C Activations with Zwitterionic Bis-phospholane Ligands

Nicolai Cramer

The development of unconventional ligand scaffolds is an important aspect to alter reaction pathways of transition-metal-catalyzed reactions. The nature of the counterion of cationic metal complexes plays an important role in the catalyst reactivity. We he ...

Amer Chemical Soc2014

Electronic Elements Governing the Binding of Small Molecules to a [Fe]-hydrogenase Mimic

Matthew Wodrich, Xile Hu

[Fe]-hydrogenase, one of three types of hydrogenases, activates molecular hydrogen. Here, using DFT computations, we examine the electronic elements governing the binding of small ligands to a recently synthesized [Fe]-hydrogenase biomimic. Computed reacti ...

Wiley-Blackwell2013

Reversible protonation of a thiolate ligand in an [Fe]-hydrogenase model complex

Rosario Scopelliti, Xile Hu, Dafa Chen

The thiolate ligand in the five-coordinate model complex 1 of [Fe]-hydrogenase is preferentially and reversibly protonated, even in the presence of an acyl ligand. The results suggest that the Cys176 thiolate ligand in [Fe]-hydrogenase can serve as the int ...

Wiley-VCH Verlag GmbH2012

Design and Development of Functionalized Cyclometalated Ruthenium Chromophores for Light-Harvesting Applications

Michael Graetzel, Mohammad Khaja Nazeeruddin, Thomas Baumgartner, Aswani Yella

The syntheses and the electrochemical spectroscopic properties of a suite of asymmetrical bistridentate cyclometalated Ru(II) complexes bearing terminal triphenylamine (TPA) substituents are reported. These complexes, which contain structural design elemen ...

2011

Mechanistic studies on two dinuclear organogold(III) compounds showing appreciable antiproliferative properties and a high redox stability

Angela Casini

Two dinuclear oxo-bridged organogold(III) compounds, namely [(N,N,C)(2)Au-2(mu-O)]PF6 (with N,N,CH = 6-(1-methylbenzyl)-2,2'-bipyridine, Au(2)O1; or 6-(1,1-dimethylbenzyl)-2,2'-bipyridine, Au(2)O2), were previously prepared and characterised. Their so ...

2011

Synthesis and Reactivity of Iron Acyl Complexes Modeling the Active Site of [Fe]-Hydrogenase

Rosario Scopelliti, Xile Hu, Dafa Chen

A [FeIIFeII] dithiolate complex containing acyl and carbonyl ligands was synthesized. The diiron complex reacted with phosphine, cyanide, isocyanide, and CO to give monomeric FeII complexes reproducing the first coordination sphere of the active site of [F ...

2010

Anticancer activity of new organo-ruthenium, rhodium and iridium complexes containing the 2-(pyridine-2-yl)thiazole N,N-chelating ligand

Paul Joseph Dyson, Angela Casini, Fabio Edafe

The dinuclear dichloro complexes [(η6-arene)2Ru2(μ-Cl)2Cl2] and [(η5-C5Me5)2M2(μ-Cl)2Cl2] react with 2-(pyridine-2-yl)thiazole (pyTz) to afford the cationic complexes [(η6-arene)Ru(pyTz)Cl]+ (arene = C6H6 (1), p-iPrC6H4Me (2) or C6Me6 (3)) and [(η5-C5Me5)M ...

Elsevier2010

Understanding the Effect of Magnesium Ion Concentration on the Catalytic Activity of Ribonuclease H through Computation: Does a Third Metal Binding Site Modulate Endonuclease Catalysis?

Matteo Dal Peraro

Ribonuclease H (RNase H) belongs to the nucleotidyl-transferase superfamily and hydrolyzes the phosphodiester linkage on the RNA strand of a DNA/RNA hybrid duplex. Due to its activity in HIV reverse transcription, it represents a promising target for anti- ...

2010