Article
Chemistry, Multidisciplinary
Mengfei Wang, Kei Murata, Yosuke Koike, Gediminas Jonusauskas, Amaury Furet, Dario M. Bassani, Daisuke Saito, Masako Kato, Yuushi Shimoda, Kiyoshi Miyata, Ken Onda, Kazuyuki Ishii
Summary: A recent study has demonstrated the photo-induced CO-releasing capabilities of the complex Re1Pc, which is composed of a [Re(CO)(3)](+) unit and a phthalocyanine ligand. The complex exhibited efficient spin-orbit coupling and large Franck-Condon factors, resulting in short excited-state lifetimes and ultrafast intersystem crossing. This research provides promising insights into the development of red-light-driven photoCORMs for biomedical applications.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Julia G. Knapp, Maksim Y. Livshits, J. Connor Gilhula, Sylvia L. Hanna, Ida D. Piedmonte, Natalie T. Rice, Xingjie Wang, Benjamin W. Stein, Stosh A. Kozimor, Omar K. Farha
Summary: This study investigated the impact of linker identity and photoexcitation on the photocatalytic performance of uranyl-based MOFs. By analyzing the structural and photochemical properties of three uranyl-based MOFs, the study showed that the photophysical properties of linkers can be used to predict the photocatalytic behavior of uranyl-containing MOFs.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Christopher Thomas, Marina Wittig, Bernhard Rieger
Summary: The new supramolecular photocatalyst RuRe3 shows high activity and photostability in reducing CO2 to CO. The efficient second electron transfer mechanism and intermolecular electron transfer contribute to the superior performance of this tetranuclear complex. Further studies on these synergistic effects could lead to the design and synthesis of new and efficient supramolecular CO2-reducing photocatalysts.
Article
Chemistry, Multidisciplinary
Maximilian Fritz, Severine Rupp, Ciara I. Kiene, Sesha Kisan, Joshua Telser, Christian Wurtele, Vera Krewald, Sven Schneider
Summary: This study presents a new method for the conversion of dinitrogen to benzonitrile, which involves photoelectrochemical reduction of N-2 followed by N-benzoylation to achieve selective nitrogen transfer and produce nitrogenous organic products in photoelectrosynthesis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Chemistry, Multidisciplinary
Pietro Franceschi, Sara Cuadros, Giulio Goti, Luca Dell'Amico
Summary: The synthesis of four-membered heterocycles often requires complex procedures and prefunctionalized reactants. An alternative approach is the photochemical [2+2]-heterocycloaddition, but it is limited by the absorption profile of the carbonyl and the use of high-energy UV-light. This review highlights the progress made in developing visible light-driven [2+2]-heterocycloadditions and discusses the remaining challenges and potential future directions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Han Li, Oliver S. Wenger
Summary: Our study demonstrates the concept that single excitation of the two-electron reduced forms of perylene diimides (PDIs) with green photons can produce excited states with similar or greater reducing power than the shorter-lived excited states of PDI radical monoanions. By performing multi-electron reduction of a photocatalyst with a sacrificial reagent before irradiation with low-energy photons, we can generate highly reactive excited states for photocatalytic reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Nanoscience & Nanotechnology
Jacob B. Khurgin, Alexander Petrov, Manfred Eich, Alexander Uskov
Summary: Research on plasmon-driven chemical reactions explores a new pathway of direct excitation of hybridized surface states, which can potentially achieve a rate comparable to or exceeding that of indirect excitation. These findings contribute to optimizing plasmon-driven photochemistry and bringing it closer to practical applications.
Article
Chemistry, Multidisciplinary
Huyan Zhou, Lu Zhang, Peng Wen, Yang Zhou, Yucheng Zhao, Qiaoqiao Zhao, Yu Gu, Ruopeng Bai, Mao Chen
Summary: In this study, photoredox-mediated reversible-deactivation radical polymerization (RDRP) was developed by activating (hetero)aryl sulfonyl chloride (ArSO2Cl) initiators with pyridines and designing a novel bis(phenothiazine)arene catalyst. The in situ formed sulfonyl pyridinium intermediates effectively promote controlled chain-growth from ArSO2Cl, enabling access to various well-defined polymers with high initiation efficiencies and controlled dispersities under mild conditions. This versatile method allows ON/OFF temporal control, chain-extension, and facile synthesis of different polymer brushes via organocatalyzed grafting reactions from linear chains. Time-resolved fluorescence decay studies and calculations support the reaction mechanism. This work provides a transition-metal-free RDRP to tailor polymers with readily available aromatic initiators, and will promote the design of polymerization leveraged from photoredox catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Lavinia A. Trifoi, Nicholas P. Dogantzis, Gregory K. Hodgson, Pedro D. Ortiz, Sumaiya A. Soha, Costin N. Antonescu, Roberto J. Botelho, R. Stephen Wylie, Stefania Impellizzeri
Summary: We synthesized a fluorogenic methylated dihydrofluorescein derivative that can be activated and fluoresce under visible-light illumination. This study provides a simple optical method to simultaneously activate and excite fluorescence using a single wavelength, and the fluorescence can be further enhanced through metal-enhanced fluorescence.
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Johannes Grosskopf, Thorsten Bach
Summary: Upon irradiation with a suitable chiral catalyst, racemic compounds can be converted into enantiopure compounds through a process called photochemical deracemization. This review comprehensively covers the research and current developments in this field, discussing the reactions and mechanistic details underlying the presented reaction. Photochemical deracemization offers a unique opportunity to directly obtain enantiopure compounds from racemates, and short-lived intermediates play a key role in determining the enantioselectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Linan Zhou, Minhan Lou, Junwei Lucas Bao, Chao Zhang, Jun G. Liu, John Mark P. Martirez, Shu Tian, Lin Yuan, Dayne F. Swearer, Hossein Robatjazi, Emily A. Carter, Peter Nordlander, Naomi J. Halas
Summary: This study demonstrates that the H2-D2 exchange reaction catalyzed by Cu nanoparticles is primarily driven by thermalized hot carriers, with an intriguing intensity-dependent external quantum yield exceeding 100% at high light intensities. Quantum mechanical research suggests that vibrational excitations of the surface Cu-H bond are the likely activation mechanism, supporting the effectiveness of low-energy thermalized hot carriers in photocatalyzing this reaction.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Review
Chemistry, Inorganic & Nuclear
Hande Gunduz, Safacan Kolemen, Engin U. Akkaya
Summary: The detection and imaging of singlet oxygen is a challenging task due to its short half-life and solvent sensitivity. Selective probes for singlet oxygen are crucial in the presence of other oxidizing species, and smart designs are already making progress in pushing signalling events towards longer wavelengths of the visible spectrum.
COORDINATION CHEMISTRY REVIEWS
(2021)
Article
Chemistry, Physical
Alexandre Jacques, Alexandre Devaux, Christophe Rubay, Florence Pennetreau, Antonin Desmecht, Koen Robeyns, Sophie Hermans, Benjamin Elias
Summary: Iridium(III) and ruthenium(II) polypyridyl based photocatalysts were synthesized and characterized, with their structures determined using H-1 NMR, HR-MS and single crystal XRD techniques. Their spectroscopic and electrochemical properties were investigated using UV-vis absorption, emission spectroscopy and cyclic voltammetry. These complexes were utilized as photoredox homogeneous catalysts in an intramolecular cyclization reaction, exhibiting high activity. They were immobilized on graphene oxide (GO) via esterification and non-covalently attached to reduced graphene oxide (rGO) through pyrene moieties. The heterogenized complexes showed good photocatalytic activity, and notably, the use of a pyrene-derivatized Ir(III) terpyridine-based complex revealed an unexpected on/off effect of the photocatalytic activity depending on the presence or absence of rGO.
Review
Chemistry, Multidisciplinary
Alberto Vega-Penaloza, Javier Mateos, Xavier Companyo, Margarita Escudero-Casao, Luca Dell'Amico
Summary: Organic photocatalysts are proving to be more sustainable tools compared to metal complexes, with recent advancements in applications and structural redesign. Rational structural modification of these photocatalysts is crucial for achieving unprecedented reactivity and enhancing their catalytic performances by altering physicochemical and redox properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Robin Giereth, Philipp Lang, Ewan McQueen, Xenia Meissner, Beatrice Braun-Cula, Carla Marchfelder, Martin Obermeier, Matthias Schwalbe, Stefanie Tschierlei
Summary: Researchers synthesized a homobimetallic rhenium(I) compound that significantly increased catalytic performance, and shed light on crucial intermediates in the reaction cycle through photocatalytic experiments, spectroelectrochemical experiments, and spectroscopic investigations under (photo)catalytic conditions.
Review
Chemistry, Analytical
Lucyano J. A. Macedo, Fernando P. Rodrigues, Ayaz Hassan, Leandro N. C. Maximo, Fabio Zobi, Roberto S. da Silva, Frank N. Crespilho
Summary: Recent emergence of FTIR spectromicroscopy (micro-FTIR) as a dynamic spectroscopy for imaging to study biological chemistry has opened new possibilities for investigating in situ drug release, redox chemistry effects on biological molecules, DNA and drug interactions, membrane dynamics, and redox reactions with proteins at the single cell level. Micro-FTIR applied to metallodrugs has been playing an important role since the last decade because of its great potential to achieve more robust and controlled pharmacological effects against several diseases, including cancer. An important aspect in the development of these drugs is to understand their cellular properties, such as uptake, accumulation, activity, and toxicity. The review highlights both the potential application of micro-FTIR and its importance for studying metal-based drugs, emphasizing the perspectives of chemistry of living cells and the significance of bioimaging for localization of cellular processes to understand the mechanism of action.
ANALYTICAL METHODS
(2022)
Review
Biochemistry & Molecular Biology
Kevin Schindler, Fabio Zobi
Summary: Organometallic compounds of rhenium, particularly its tri- and dicarbonyl complexes, have shown promising potential as anticancer and antibiotic drugs due to their ease of preparation, stability, and unique photophysical and luminescent properties. This review focuses on discussing the structural variations and in vitro efficacy of these complexes in the past seven years, with an initial emphasis on tricarbonyl complexes and a later discussion on the future prospects of dicarbonyl species in this field.
Article
Multidisciplinary Sciences
Hagir B. Suliman, Zachary Healy, Fabio Zobi, Bryan D. Kraft, Karen Welty-Wolf, Joshua Smith, Christina Barkauskas, Claude A. Piantadosi
Summary: The preclinical model of bleomycin-induced lung fibrosis is useful to study mechanisms related to human pulmonary fibrosis. The study found that HO-1/NRF-1 signaling protects lung AT2 cells against injury and fibrosis by maintaining mitochondrial health and suppressing the TGF beta 1 pathway.
Article
Biochemistry & Molecular Biology
Sara Nasiri Sovari, Taryn M. Golding, Mziyanda Mbaba, Roxanne Mohunlal, Timothy J. Egan, Gregory S. Smith, Fabio Zobi
Summary: A small library of aminoquinoline and imidazolopiperidine (IMP)-based ligands showed potent inhibitory activities against chloroquine-sensitive (CQS) and multidrug-resistant (MDR) strains of P. falciparum. The compounds may act through hemozoin inhibition and the quinoline-based compounds exhibited higher binding affinities than the reference drug chloroquine.
JOURNAL OF INORGANIC BIOCHEMISTRY
(2022)
Article
Chemistry, Medicinal
Kevin Schindler, Youri Cortat, Miroslava Nedyalkova, Aurelien Crochet, Marco Lattuada, Aleksandar Pavic, Fabio Zobi
Summary: Antimicrobial resistance poses a significant threat to human health and has a major impact on the global economy. Metal complexes, including rhenium complexes, have untapped potential as antimicrobial agents. This study investigates the antimicrobial potential of rhenium di- and tricarbonyl diimine complexes and identifies two potential targets for these compounds. The findings have implications for the future design of rhenium tricarbonyl diimine-based antibiotics.
Article
Chemistry, Organic
Fatlinda Rahmani, Aurelien Crochet, Fabio Zobi
Summary: In this study, (E)-3-(2-(4-methylthiazol-2-yl)hydrazineylidene)chromane-2,4-dione was synthesized for the first time and characterized using various spectroscopic techniques. The chemical structure and isomeric configuration of the molecule were confirmed by single-crystal X-ray diffraction.
Article
Infectious Diseases
Youri Cortat, Miroslava Nedyalkova, Kevin Schindler, Parth Kadakia, Gozde Demirci, Sara Nasiri Sovari, Aurelien Crochet, Stefan Salentinig, Marco Lattuada, Olimpia Mamula Steiner, Fabio Zobi
Summary: In the context of the global health issue caused by antimicrobial resistance (AMR), the need for novel antimicrobial agents is urgent. Inorganic and organometallic complexes show potential as untapped sources of antibiotics. This study used a computer-aided drug design approach to synthesize and evaluate fac-Re(I) tricarbonyl complexes as antibacterial agents, with promising results.
Article
Chemistry, Inorganic & Nuclear
Kevin Schindler, Justine Horner, Gozde Demirci, Youri Cortat, Aurelien Crochet, Olimpia Mamula Steiner, Fabio Zobi
Summary: Cancer is still a leading cause of death worldwide, and the interest in organometallic complexes as anticancer drug candidates is crucial. Rhenium dicarbonyl complexes have been given less attention compared to tricarbonyl complexes. This study tested various rhenium dicarbonyl complexes in vitro against different cancer cell lines and found that some compounds showed good activity against specific cancer lines but were also toxic to healthy cells.
Review
Pharmacology & Pharmacy
Youri Cortat, Fabio Zobi
Summary: This review discusses the research work on coordination derivatives of antifungal azoles (AAs) synthesized for medical purposes, highlighting the most promising compounds and emphasizing the efficiency of AAs and their metallic species.
Article
Chemistry, Inorganic & Nuclear
Sara Nasiri Sovari, Isabelle Kolly, Kevin Schindler, Ana Djuric, Tatjana Srdic-Rajic, Aurelien Crochet, Aleksandar Pavic, Fabio Zobi
Summary: This study reports the synthesis, characterization, and in vivo evaluation of a series of rhenium tricarbonyl complexes containing 5- and 6-(halomethyl)-2,2'-bipyridine ligands. The aim was to investigate the role of a reactive halomethyl substituent on the diimine ligand system in the design of effective and non-toxic anticancer agents. Compounds capable of undergoing ligand-based alkylating reactions exhibited significant antiproliferative activity against colorectal and pancreatic cell lines. One specific compound (5-(chloromethyl)-2,2'-bipyridine derivative) displayed significant inhibition of pancreatic tumor growth in vivo in zebrafish-Panc-1 xenografts at a concentration of 8 μM, lower than its in vitro IC50 values, and also inhibited in vivo cancer cell dissemination.
DALTON TRANSACTIONS
(2023)